Physical Crosslinking Research Articles

Preparation of chitin twisted fiber and its functional applications

Chitin has garnered significant attention due to its renewable, biocompatibility and biodegradability, while its practical application seriously hindered as the functionality of chitin itself can no longer meet people's increasing requirements for materials. Here, an effective method is successfully built for high-performance chitin fibers fabrication through a multi-step strategy that involved chemical pre-crosslinking, followed by wet-twisting and wet-stretching techniques, combined with physical cross-linking. The as-prepared chitin fiber exhibited a smooth surface, adjustable diameter, and mechanical strong properties (144.6 MPa). More importantly, functional chitin fiber with magnetic or conductive abilities can be easily obtained by spraying Fe3O4 particles or Ag nanowire on the chemical pre-crosslinking chitin gel film before stretching and twisting. The doped functional inorganic particles exist in a continuous ribbon structure in the fiber reduced the decrease in material strength caused by uneven particles dispersion, resulting 88.4 % of stress and 91.6 % of strain retention. This work not only bestow invaluable insights into the fabrication of functional chitin fibers but also provide a novel approach to solve the problem of poor compatibility between organic and inorganic composite materials.

A super-stretchable and anti-fatigue silicone gel by regulating chain entanglement and cross-link density

Applications of silicone gel in flexible devices and soft machines require it to maintain excellent stretchability and antifatigue. However, the reported fatigue threshold of traditional silicone gels is in the range of 1–100 J m−2 and the stretchability below 2000 %. Herein, we report a simple strategy for constructing soft polydimethylsiloxane gels, which possesses high stretchability up to 8300 %, and high fatigue resistance (321 J m−2). This is achieved by controlling the ratio of chemical crosslinking and physical entanglement in the polydimethylsiloxane gels. The symbiotic relationship of this combination includes: extending the polymer chains helps them unfold to increase softness and intrinsic toughness; controlling the physical entanglement and chemical cross-linking helps to further increase the tensile rate and fatigue threshold, and adding small-molecule dimethyl PDMS as a solvent further increases fatigue resistance and tensile properties. This work provides a facile approach for developing super-stretchable and anti-fatigue silicone gel, which promises wide range of applicant in flexible devices and soft machines.

Triple-crosslinked double-network alginate/dextran/dendrimer hydrogel with tunable mechanical and adhesive properties: A potential candidate for sutureless keratoplasty

An ideal adhesive hydrogel must possess high adhesion to the native tissue, biocompatibility, eligible biodegradability, and good mechanical compliance with the substrate tissues. We constructed an interpenetrating double-network hydrogel containing polysaccharides (alginate and dextran) and nanosized spherical dendrimer by both physical and chemical crosslinking, thus endowing the hydrogel with a broad range of mechanical properties, adhesive properties, and biological functions. The double-network hydrogel has moderate pore sizes and swelling properties. The chelation of calcium ions significantly enhances the tensile and compressive properties. The incorporation of dendrimer improves both the mechanical and adhesive properties. This multicomponent interpenetrating network hydrogel has excellent biocompatibility, tunable mechanical and adhesive properties, and satisfied multi-functions to meet the complex requirements of wound healing and tissue engineering. The hydrogel exhibits promising corneal adhesion capabilities in vitro, potentially supplanting the need for sutures in corneal stromal surgery and mitigating the risks associated with donor corneal damage and graft rejection during corneal transplantation. This novel polysaccharide and dendrimer hydrogel also shows good results in sutureless keratoplasty, with high efficiency and reliability. Based on the clinical requirements for tissue bonding and wound closure, the hydrogel provides insight into solving the mechanical properties and adhesive strength of tissue adhesives.

Temperature- and pH-induced dual-crosslinked methylcellulose/chitosan-gallol conjugate composite hydrogels with improved mechanical, tissue adhesive, and hemostatic properties

Gauze or bandages are commonly used to effectively control bleeding during trauma and surgery. However, conventional treatment methods can sometimes lead to secondary damages. In recent years, there has been increased interest in developing adhesive hemostatic hydrogels as a safer alternative for achieving hemostasis. Methylcellulose (MC) is a well-known thermo-sensitive polymer with excellent biocompatibility that is capable of forming a hydrogel through physical crosslinking owing to its inherent thermo-reversible properties. However, the poor mechanical properties of the MC hydrogel comprising a single crosslinked network (SN) limit its application as a hemostatic material. To address this issue, we incorporated a chitosan-gallol (CS-GA) conjugate, which has the ability to form chemical crosslinks through self-crosslinking reactions under specific pH conditions, into the MC hydrogel to reinforce the MC hydrogel network. The resulting MC/CS-GA hydrogel with a dual-crosslinked network (DN), involving both physical and chemical crosslinks, exhibited synergistic effects of the two types of crosslinks. Thus, compared with those of the SN hydrogel, the composite DN hydrogel exhibited significantly enhanced mechanical strength and tissue adhesive properties. Moreover, the DN hydrogel presented excellent biological activity in vitro. Additionally, in rat hepatic hemorrhage models, the DN hydrogel exhibited high hemostatic efficiency, showcasing its multifunctional capabilities.

Bio-inspired stretchable and self-healable nanocomposite gelatin hydrogel with low silica nanoparticle content and brilliant angle/strain-independent structural colors

Stretchable and self-healable structural-colored nanocomposite gelatin hydrogel with photonic structure of random dense/loose regions of non-close-packed silica nanoparticles (SiO2 NPs) is developed via convenient and scalable polymer-mediated assembly. The formation of the special photonic structure with overall low SiO2 NP content is characterized by transmission electron microscopy (TEM) and scanning electron microscopy (SEM). The small-angle X-ray scattering test indicates the existence of short-range order, which is consistent with the TEM and SEM results. The dense photonic structure consisting of SiO2 NP chains and domains, and the loose structure consisting of abundant solitary SiO2 NPs, accounts for pronounced and uniform structural colors via combined effects of coherent scattering of light by dense structure, and Mie scattering of solitary NPs. These structural colors are independent of viewing angles and large mechanical strains. The dynamic physical and chemical bonding of the gelatin hydrogel network matrix enables self-healing functions and good deformability. Moreover, salt treatment of the structural-colored gelatin hydrogel networks enhances physical crosslinking and the mechanical strength of the hydrogel. The resilient, flexible and self-healable structural-colored nanocomposite hydrogel with low SiO2 NP content has great potential in wearable photonics, cosmetics, and various other color-related fields. This work also sheds light on enhancing non-iridescent structural colors through advanced photonic design.

Structure and thermal properties of acrylic copolymer gels: effect of composition and cross-linking method

Two approaches to the synthesis of hydrogels based on polyacrylamide (pAAm) with copolymers were compared in the paper—traditional chemical cross-linking and physical cross-linking with montmorillonite (MMT). The main aim of the work was to find an adequate replacement of the chemical toxic cross-linking agent MBAAm (N,N'-methylene-bis-acrylamide) by using non-toxic—natural clay MMT for synthesis of pAAm gels, which are planned to be used as soil conditioners. A series of hydrogels based on acrylic monomers (acrylamide (AAm), acrylonitrile (AN), acrylic acid (AA)) physically cross–linked by MMT and chemically cross-linked were synthesized. For the synthesized gels, the influence of the synthesis method on the formation of the structure and the mechanism of thermal destruction in the presence of air was analyzed using a set of physicochemical methods: FTIR, XRD, SEM, DSC and TG/DTG. According to FTIR and XRD data, pAAm-MMT and pAAm-AN-MMT samples formed an intercalated/exfoliated structure, whereas pAAm-AA-MMT had an intercalated structure. The endothermic reaction of decomposition of xerogels based on acrylic polymers with and without MMT was observed using DSC and derivative thermogravimetry analyses, coupled with measurement of FTIR spectra of volatile products of thermolysis. All studied composites were relatively thermoresistant, which had three distinct regions of phase transitions and their thermal decomposition occurred at a temperature range 310–465 °C.Graphical

Agaricus blazei Murill extract-loaded alginate/poly (vinyl alcohol)-based microgels as potential wound dressings

The development of new biomaterials based on natural products for wound treatment is a frequent research topic in recent years. In this study, the hydroalcoholic extract from Agaricus blazei Murill (EAb) was incorporated in microgels based on poly (vinyl alcohol) (PVA) and sodium alginate (SA). Microgels were characterized according to their physicochemical and morphological properties. An in vivo wound healing assay was performed and histomorphometric parameters and oxidative stress were studied. The physicochemical characterizations showed the occurrence of intermolecular interactions between both polymers and this natural product, suggesting a potential physical cross-linking. The microgels presented sol-gel transition (G’ > G’’) at low frequencies, porosity degree around 40 % and significant ability to scavenge the DPPH radical. Morphological characterization evidenced pores on the micrometric scale, where EAb granules (0.3–0.6 µm) are trapped. On the 14th day, mice treated with EAb-loaded microgels presented wound contraction > 99 %, as well as greater epidermis and dermis thickness, higher density of type I collagen and significant reduction in oxidative stress. Our results showed that EAb-loaded microgels, especially the M0.5 formulation, are a promising multifunctional biomaterial for wound dressing applications.

Neural network inspired bionic ordered structure polyaniline gel for wearable sensor

In recent years, remarkable progress has been made in the research and development of traditional conductive polymer gel wearable sensors. However, it is still a challenge to achieve high sensitivity and mechanical strength at the same time due to the influence of the characteristics of conductive material in gels. Herein, inspired by human neural network, a novel biomimetic ordered polyaniline conductive gel is presented with stable conductivity (18.04 S/m), excellent sensitivity (GF of 3.53) under the condition of high elongation (stretching of 400 %-500 %), good mechanical properties, biocompatibility, and anti-freezing performance. This conductive gel is composed of maleic anhydride modified γ-cyclodextrin, polyaniline, and polyacrylamide. Modified γ-cyclodextrin can be firmly fixed on the polyacrylamide skeleton of the gel through chemical bonds. The aniline is evenly distributed in the hydrophobic cavity of modified cyclodextrin through hydrophobic interaction, and an ordered polyaniline network with γ-cyclodextrins as a physical crosslinking point is formed in the gel. This biomimetic ordered structure greatly improves the toughness and conductivity of the polyaniline network, which significantly enhances the sensing ability of polyaniline gels. This work is expected to provide a novel method for improving the mechanical and electrical properties of polyaniline gels and pave an avenue for the uniform dispersion of non-polar substances in polar gels.

Fabrication of black wolfberry anthocyanin-based hydrogels for monitoring freshness and extending shelf-life of Dolang lamb

In this study, a black wolfberry anthocyanin-based indication label (BWIL) was developed using black wolfberry pigment (BWP) in combination with polyvinyl alcohol (PVA) and carboxymethyl cellulose (CMC) (PVA:CMC = 4:3). The potential use of BWIL for monitoring the freshness of Dorang lamb was further investigated. As revealed, physical cross-linking occurred between PVA, CMC and BWP during the preparation of BWIL. The addition of BWP promoted the internal cross-linking, porosity, and thermal stability of BWIL significantly (p < 0.05). Specifically, BWIL showed a distinct color change when exposed to the refrigerated conditions of Dorang lamb. After 6 days, 12 days and 16 days of lamb refrigeration, the ΔE of BWIL was 26.3, 28.6 and 30.7, respectively, which far exceeded the human eyes' color threshold discernible (ΔE = 3.5). Besides, the ΔE of BWIL was significantly correlated with pH, fat oxidation, and TVB-N content of Dorang lamb (p < 0.05). This result indicated that BWIL could be used for identifying the freshness of lamb accurately. Importantly, the shelf-life of lamb with BWIL was extended from 6 days to 16 days, which suggests that BWIL would be an effective tool for real-time freshness monitoring and shelf-life extending of Dorang lamb.

Biomimetic kartogenin containing κ-carrageenan hydrogel for nucleus pulposus regeneration

Intervertebral disc degeneration is a clinical disease that reduces the quality of patient's life. The degeneration usually initiates in the nucleus pulposus (NP), hence the use of hydrogels represents a promising therapeutic approach. However, the viscoelastic nature of hydrogel and its ability to provide biomimetic architecture and biochemical cues influence the regeneration capability. This study focused on tuning the physical nature of a glycosaminoglycan hydrogel (κ-carrageenan) as well as the release kinetics of a chondrogenic factor (kartogenin - KGN) through physical cross-linking. For this, κ-carrageenan was cross linked with 2.5 % and 5 % potassium chloride (KCl) for 15 and 30 min and loaded with KGN molecule at 50 μM and 100 μM. The tight network structure with low water retention and degradation property was seen in hydrogel cross-linked with increased KCl concentration and time. However, optimal degradation along with NP mimicking viscoelastic nature was exhibited by 5 wt% KCl treated hydrogel (H3 hydrogel). All hydrogel groups exhibited burst KGN release at 24 h followed by a sustained release for 5 days. However, hydrogel cross-linked with 5 wt% KCl enhanced chondrogenic differentiation, mainly at lower KGN dose. In summary, this study shows the potential application of biomimetic KGN laden carrageenan hydrogel in NP regeneration.

Multi-Layer PVA-PANI Conductive Hydrogel for Symmetrical Supercapacitors: Preparation and Characterization.

This work describes a simple, inexpensive, and robust method to prepare a flexible "all in one" integrated hydrogel supercapacitors (HySCs). Preparing smart hydrogels with high electrical conductivity, ability to stretch significantly, and excellent mechanical properties is the last challenge for tailored wearable devices. In this paper, we employed a physical crosslinking process that involves consecutive freezing and thawing cycles to prepare a polyvinyl alcohol (PVA)-based hydrogel. Exploiting the self-healing properties of these materials, the assembly of the different layers of the HySCs has been performed. The ionic conductivity within the electrolyte layer arises from the inclusion of an H2SO4 solution in the hydrogel network. Instead, the electronic conductivity is facilitated by the addition of the conductive polymer PANI-PAMPSA into the hydrogel layers. Electrochemical measures have highlighted newsworthy properties related to our HySCs, opening their use in wearable electronic applications.

Fabrication of polydopamine-modified cellulose hydrogel for controlled release of α-mangostin.

Hydrogels are notable for their outstanding absorbent qualities, satisfactory compatibility with biological systems, ability to degrade, and inherent safety, all of which contribute to their high demand in the field of biomedicine. This study focuses on the fabrication of hydrogels using environmentally friendly cellulosic material. Cellulose hydrogel beads were prepared by physical cross-linking in a NaOH/urea medium. Furthermore, nano polydopamine was integrated into the hydrogel matrix as functional polymers and α-mangostin was employed as an active pharmaceutical ingredient. The physicochemical properties were comprehensively analyzed using Fourier-transform infrared spectrometer, 13C cross-polarization/magic angle spinning nuclear magnetic resonance, thermogravimetric analysis, and scanning electron microscope. The drug delivery properties, including water content, swelling ratio, and drug release profiles, were evaluated. In vitro cytotoxicity against MC3T3-E1 cells was assessed using sulforhodamine B staining. All test hydrogels exhibited inhibitory activity against the growth of MC3T3-E1 cells. These results indicated the potential use of these hydrogels as a drug delivery carrier for α-mangostin in the treatment of ankylosing spondylitis.

Supramolecular hydrogels based on hydrogen bonding: Impact of ionic comonomers

AbstractThe polymerization of N‐acryloyl glycineamide (NAGA) in water results in the creation of robust supramolecular hydrogels, exhibiting a network structure through inter‐chain crosslinking formed by hydrogen bonds between NAGA units. The stability of these hydrogen bonds in water is based on the aggregation of NAGA units into microdomains or clusters, thereby effectively shielding the hydrogen bonds from the surrounding aqueous medium. Beyond the inherent water absorption characteristics of these hydrogels, the unique ability for the dissociation and re‐association of their physical crosslinks imparts features such as reversible swelling and shrinking as well as self‐healing and remolding capabilities. In this study, we synthesize a series of supramolecular hydrogels through copolymerization of NAGA and ionic sodium acrylate comonomers for a dual purpose: first, to regulate water absorption levels, and second, to introduce a salt partitioning effect into the hydrogels during their swelling in salt solution. Our findings indicate that the properties of these hydrogels are intricately influenced by the volume fraction of the solid network, the concentration of ionic units, and temperature. Notably, supramolecular samples with ionic units exhibit a 16% salt rejection in a single cycle of salt partitioning during their swelling in a 1 g·L−1 sodium chloride solution.

DEVELOPMENT OF ZINC-LOADED HYDROGEL INFUSED WITH ALOE BARBADENSIS MUCILAGE FOR WOUND HEALING

This study aims to formulate and characterize zinc-loaded hydrogel infused with Aloe barbadensis mucilage for wound dressing. Five formulations containing varying proportions of carbopol, zinc, aloe and water (as vehicle) were developed via physical crosslinking using triethanolamine. All formulations had a translucent off-white colour while the control gave a transparent gel. The viscosity was highest in the control, 30000.00 ± 2.07 PaS. The pH of the formulations was between 5.7 and 5.8. Formulation 2 which is composed of 30 mg of Zinc and 1.4 mg of Aloe barbadensis incorporated into 1% w/v Carbopol Ultrez hydrogel polymer had the lowest swelling index of 79.2 ± 1.95% implying that it had the fastest drug release rate. The wounds treated with Formulation 2 had the most rapid wound healing with no sign of scars in the wound area. Histomorphometric evaluation reflected a high re-epithelisation rate of 70%, a significant percentage occupied by collagen in granulation tissue of 85%. The thickness of the tissue's central region was 10 mm. The inflammatory cells /mm2 tissue was 200 cells/mm2 while the number of microvessels in granulation tissue was 1.0 microvessels/mm2. Zinc-loaded hydrogel infused with Aloe barbadensis mucilage shows great potential as a modern wound dressing.

Solvent-free polyurethane adhesives with excellent adhesion performance at ultra-low temperature

Adhesives with excellent adhesion and high elongation at cryogenic temperatures are necessary for fields such as aerospace, transportation, superconductors, and medicine, but have difficult requirements. This study aimed to develop a solvent-free, two-component polyurethane (PU) adhesive with excellent adhesion and high elongation, especially in ultra-low temperature conditions. we incorporated bulky polydimethylsiloxane (PDMS) diol into the hard segment of the PU adhesive to enhance flexibility and improve physical cross-linking within the adhesive matrix. The resulting PDMS-based PU adhesive showed a tensile strength of 120 MPa at −170 °C and a high elongation of approximately 4 %. It showed a lap-shear strength of up to 13 MPa at −196 °C. Additionally, the adhesive was curable at 23 °C. In this study, the cryogenic applicability of the PU adhesive was evaluated at −170 °C (103 K, liquid natural gas) and −196 °C (77 K, liquid nitrogen). Future research on the polymer adhesive materials applicable to ultra-low temperatures, such as 20 K, may be necessary if storage and transportation of liquid hydrogen become feasible.

Mechanical and viscoelastic properties of novel resin-infused thermoplastic tri-block copolymer 3D glass fabric composites

The current study investigates the mechanical and viscoelastic properties of a novel acrylic resin-infused thermoplastic (Elium®) tri-block copolymer (Nanostrength®) 3D fibre-reinforced composites (FRCs). The toughened thermoplastic resins with three different concentrations of tri-block copolymer, i.e., 10 wt%, 15 wt%, and 20 wt%, were prepared and used to fabricate thermoplastic 3D-FRCs using a vacuum-assisted resin-infusion process at room temperature. The flexural, interlaminar, and viscoelastic properties and failure modes were evaluated and compared with those of pristine thermoplastic 3D-FRCs. The addition of tri-block copolymer significantly improves the flexural strength of 3D-FRC (up to 75 % and 34 % along the warp and fill directions, respectively, at 15 wt% of tri-block copolymer) and interlaminar shear strength (up to 80 % and 111 % along the warp and fill directions, respectively, at 20 wt% of tri-block copolymer). Additionally, the residual flexure and interlaminar shear strength improved up to 35 % and 109 % at 15 wt% of tri-block copolymer. Dynamic mechanical analysis (DMA) demonstrated that the glass transition temperature and storage modulus of thermoplastic 3D-FRCs were increased up to 11 °C and 24 %, respectively at 20 wt% of tri-block copolymer, which may be due to increased physical crosslinking and the agglomeration of tri-block copolymer particles. The improved mechanical and viscoelastic properties of resin-infused thermoplastic tri-block copolymer 3D-FRCs are attributed to better interface adhesion, improved matrix toughness, and crack-bridging mechanisms induced by the tri-block copolymer. The toughened thermoplastic 3D-FRCs can be utilized in the design and development of composite structures for improved damage tolerance applications.

Designed wrinkles for optical encryption and flexible integrated circuit carrier board

Patterns on polymers usually have different mechanical properties as those of the substrates, causing deformation or distortion and even detachment of the patterns from the polymer substrates. Herein, we present a wrinkling strategy, which utilizes photolithography to define the area of stress distribution by light-induced physical crosslinking of polymers and controls diffusion of residual solvent to redistribute the stress and then offers the same material for patterns as substrate by thermal polymerization, providing uniform wrinkles without worrying about force relaxation. The strategy allows the recording and hiding of up to eight switchable images in one place that can be read by the naked eye without crosstalk, applying the wrinkled polymer for optical anti-counterfeiting. The wrinkled polyimide film was also utilized to act as a substrate for the creation of fine copper circuit by a full-additive process. It generates flexible integrated circuit (IC) carrier board with copper wire density of 400% higher than that of the state-of-the-art in industry while fulfilling the standards for industrialization.

Phenol Removal through Horseradish Peroxidase Immobilization on Ultrafiltration Membranes: Comparative Analysis of Immobilization Methods and Fouling Patterns

This research investigates the removal of phenol using pure peroxidase from horseradish grade I in conjunction with a dead-end ultrafiltration membrane. Various horseradish peroxidase (HRP) immobilization techniques— physical adsorption, covalent bonding, and cross-linking with glutaraldehyde—were applied to a regenerated cellulose (RC) membrane with a surface area of 44 m2 and a molecular weight cut-off of 30 kDa. The investigation examined factors influencing phenol removal, including phenol concentration, membrane fouling, and the reusability of immobilized enzymes. Results indicated that covalent bonding was the most suitable enzyme immobilization technique, achieving a remarkable 90.1% immobilization yield. Phenol removal efficiency reached 100% at 30 min under specific conditions: phenol concentration of 1 mg/L, pH 6.0, hydrogen peroxide concentration of 0.5 mM, and operating pressure set at 3 psig, with temperature maintained at 28 ± 3 °C. Membrane fouling resulted in a decrease in flux. The performance of fouling models was found to be influenced by phenol concentration, with the Cake Formation Model (CFM) proving most effective at low concentrations, while the Complete Pore Blocking Model (CBM) emerged as more suitable at higher concentrations. The immobilized enzyme exhibited reusability for five cycles, maintaining a phenol removal efficiency exceeding 50%. These findings contribute to understanding the enzymatic phenol removal process and the use of appropriate enzyme immobilization techniques for the effective and sustainable treatment of phenol-contaminated water.

Viscoelastic Adhesive, Super-Conformable, and Semi-Flowable Liquid Metal Eutectogels for High-Fidelity Electrophysiological Monitoring.

Integrating gels with human skin through wearables provides unprecedented opportunities for health monitoring technology and artificial intelligence. However, most conductive hydrogels, organogels, and ionogels lack essential environmental stability, biocompatibility, and adhesion for reliable epidermal sensing. In this study, we have developed a liquid metal eutectogel simultaneously possessing superior viscoelasticity, semiflowability, and mechanical rigidity for low interfacial skin impedance, high skin adhesion, and durability. Liquid metal particles (LMPs) are employed to generate free radicals and gallium ions to accelerate the polymerization of acrylic acid monomers in a deep eutectic solvent (DES), obtaining highly viscoelastic polymer networks via physical cross-linking. In particular, graphene oxide (GO) is utilized to encapsulate the LMPs through a sonication-assisted electrostatic assembly to stabilize the LMPs in DES, which also enhances the mechanical toughness and regulates the rheological properties of the eutectogels. Our optimized semi-flowable eutectogel exhibits viscous fluid behavior at low shear rates, facilitating a highly conformable interface with hairy skin. Simultaneously, it demonstrates viscoelastic behavior at high shear rates, allowing for easy peel-off. These distinctive attributes enable the successful applications of on-skin adhesive strain sensing and high-fidelity human electrophysiological (EP) monitoring, showcasing the versatility of these ionically conductive liquid metal eutectogels in advanced personal health monitoring.

Tissue-adhesive, stretchable and compressible physical double-crosslinked microgel-integrated hydrogels for dynamic wound care

Integrated wound care through sequentially promoting hemostasis, sealing, and healing holds great promise in clinical practice. However, it remains challenging for regular bioadhesives to achieve integrated care of dynamic wounds due to the difficulties in adapting to dynamic mechanical and wet wound environments. Herein, we reported a type of dehydrated, physical double crosslinked microgels (DPDMs) which were capable of in situ forming highly stretchable, compressible and tissue-adhesive hydrogels for integrated care of dynamic wounds. The DPDMs were designed by the rational integration of the reversible crosslinks and double crosslinks into micronized gels. The reversible physical crosslinks enabled the DPDMs to integrate together, and the double crosslinked characteristics further strengthen the formed macroscopical networks (DPDM-Gels). We demonstrated that the DPDM-Gels simultaneously possess outstanding tensile (∼940 kJ/m3) and compressive (∼270 kJ/m3) toughness, commercial bioadhesives-comparable tissue-adhesive strength, together with stable performance under hundreds of deformations. In vivo results further revealed that the DPDM-Gels could effectively stop bleeding in various bleeding models, even in an actual dynamic environment, and enable the integrated care of dynamic skin wounds. On the basis of the remarkable mechanical and appropriate adhesive properties, together with impressive integrated care capacities, the DPDM-Gels may provide a new approach for the smart care of dynamic wounds. Statement of significanceIntegrated care of dynamic wounds holds great significance in clinical practice. However, the dynamic and wet wound environments pose great challenges for existing hydrogels to achieve it. This work developed robust adhesive hydrogels for integrated care of dynamic wounds by designing dehydrated, physical double crosslinked microgels (DPDMs). The reversible and double crosslinks enabled DPDMs to integrate into macroscopic hydrogels with high mechanical properties, appropriate adhesive strength and stable performance under hundreds of external deformations. Upon application at the injury site, DPDM-Gels efficiently stopped bleeding, even in an actual dynamic environment and showed effectiveness in integrated care of dynamic wounds. With the fascinating properties, DPDMs may become an effective tool for smart wound care.