Composite Hydrogel Research Articles

Multifunctional conductive composite hydrogel facilitated by high-functionality crosslinker strategy for strain sensing applications

Multifunctional conductive composite hydrogel facilitated by high-functionality crosslinker strategy for strain sensing applications

3D-Printable Gelatin Methacrylate-Xanthan Gum Hydrogel Bioink Enabling Human Induced Pluripotent Stem Cell Differentiation into Cardiomyocytes.

We describe the development of a bioink to bioprint human induced pluripotent stem cells (hiPSCs) for possible cardiac tissue engineering using a gelatin methacrylate (GelMA)-based hydrogel. While previous studies have shown that GelMA at a low concentration (5% w/v) allows for the growth of diverse cells, its 3D printability has been found to be limited by its low viscosity. To overcome that drawback, making the hydrogel both compatible with hiPSCs and 3D-printable, we developed an extrudable GelMA-based bioink by adding xanthan gum (XG). The GelMA-XG composite hydrogel had an elastic modulus (~9 kPa) comparable to that of cardiac tissue, and enabled 3D printing with high values of printing accuracy (83%) and printability (0.98). Tests with hiPSCs showed the hydrogel's ability to promote their proliferation within both 2D and 3D cell cultures. The tests also showed that hiPSCs inside hemispheres of the hydrogel were able to differentiate into cardiomyocytes, capable of spontaneous contractions (average frequency of ~0.5 Hz and amplitude of ~2%). Furthermore, bioprinting tests proved the possibility of fabricating 3D constructs of the hiPSC-laden hydrogel, with well-defined line widths (~800 μm).

Haematococcus pluvialis meets gellan gum: Rheological and thermal exploration of a new resource food and biomedical gel matrix.

The increasing interest in hydrogel matrices and their diverse applications has fueled extensive research. However, single-component gels have a limited adjustable performance range, and multi-component gels raise concerns about biological safety, hindering their widespread use. This study focuses on harnessing high-speed shearing and ultrasound-assisted methods to incorporate active natural Haematococcus pluvialis (HP), creating novel composite hydrogels in conjunction with biological macromolecule gellan gum, and eliminating the need for structural modifications or chemical crosslinking. Rich astaxanthin, proteins, polysaccharides, and other components in HP can fill and promote the formation of a unified functional network. The study aims to explore the potential of HP as a rheology regulator and investigate its impact on the rheological properties of the gels. Various rheological models, including Power-Law, Herschel-Bulkley, and Arrhenius, were employed for comparative analysis. This pioneering report on gellan/HP hydrogels holds significant importance as they exhibit optimized elasticity, thermal stability, enhanced injectability, and self-recovery, making them suitable for a wide range of applications in specialized medical food and biomedicine.

Phase-changing NIPAM-AM/ATO hydrogels for thermochromic smart windows with highly adaptive solar modulation

Improving the solar regulation and reducing the response temperature of thermochromic smart windows are pivotal importance for energy-saving buildings. However, these two strategies are challenging to be integrated into one window. Herein, a novel composite hydrogel based on N-isopropylacrylamide (NIPAM) doped with antimony-doped tin oxide (ATO) nanoparticles and acrylamide (AM) was developed for producing a high-performance smart window, which successfully achieved enhanced solar energy regulation and reduced response temperature. This smart window was fabricated by combining a reversible thermoresponsive hydrogel (TAH) that acted as a thermochromic material with a ATO multilayer film that performed as a transparent heater. The as-prepared smart window could modulate solar light over a range from ultraviolet (UV) to infrared (IR) radiation and achieved active responses to high-temperature weather. The smart window showed high luminous transmittance (Tlum, 82.92 %) together with an excellent solar modulation performance (ΔTlum = 73.31 %, ΔTIR = 38.26 %, and ΔTsol = 60.74 %), and a lower critical solution temperature of 32 °C. Even after 120 high- and low-temperature cyclic durability tests, the smart windows still exhibited a high solar modulation capability. In outdoor demonstrations, the as-prepared smart window exhibited a promising temperature regulation ability under strong solar irradiation. Therefore, the present universal modification framework provided some insights for the future design of energy-saving windows.

Comparative evaluation of adsorptive and repulsive separation using cellulose nanofiber/calcium alginate composite hydrogel filtration membranes with improved degradability

Among several approaches to address hard-to-manage dye wastewater, adsorption is one of the widely used methods, but the usage of these adsorbents can be constrained by their high material and process costs depending on the adsorbent materials as well as handling a large amount of adsorbents in a bulk solution. To overcome the problems, hydrogel membranes have recently attracted much attention because they can provide several strengths such as adsorption removal, confined adsorption sites, and filtration separation. However, to the best of our knowledge, it is still quite rare to find an in-depth comparative evaluation of adsorptive removal and repulsive separation in hydrogel membrane filtration. Herein, this study aims to bridge the gap between existing knowledge and undisclosed phenomena. Through a thorough comparative evaluation of adsorptive removal and repulsive separation in hydrogel membrane filtration, we found that repulsive separation was more suitable and sustainable than adsorptive removal because it was free from internal membrane fouling, adsorption sites’ saturation, and the cake layer formation on the surface. As a result, the hydrogel membranes could maintain excellent real-time separation performance while mitigating severe flux and rejection decline. Furthermore, we significantly improved the degradability of the spent hydrogel membrane under high saline conditions by 6.3 times compared to the control membrane by fine-tuning the structural properties via dual crosslinking, while maintaining the mechanical properties during filtration. It was possible due to the extended distance between polymer chains by dual crosslinking, reducing the burden imposed by plastic waste generated from the spent membrane.

Eco-Friendly Microwave Synthesis of Sodium Alginate-Chitosan Hydrogels for Effective Curcumin Delivery and Controlled Release.

In this study, we developed sodium alginate-chitosan hydrogels using a microwave-assisted synthesis method, aligning with green chemistry principles for enhanced sustainability. This eco-friendly approach minimizes chemical use and waste while boosting efficiency. A curcumin:2-hydroxypropyl-β-cyclodextrin complex was incorporated into the hydrogels, significantly increasing the solubility and bioavailability of curcumin. Fourier Transform Infrared Spectroscopy (FTIR) analysis confirmed the structure and successful incorporation of curcumin, in both its pure and complexed forms, into the polymer matrix. Differential scanning calorimetry revealed distinct thermal transitions influenced by the hydrogel composition and physical cross-linking. Hydrogels with higher alginate content had higher swelling ratios (338%), while those with more chitosan showed the lowest swelling ratios (254%). Scanning Electron Microscopy (SEM) micrographs showed a porous structure as well as successful incorporation of curcumin or its complex. Curcumin release studies indicated varying releasing rates between its pure and complexed forms. The chitosan-dominant hydrogel exhibited the slowest release rate of pure curcumin, while the alginate-dominant hydrogel exhibited the fastest. Conversely, for curcumin from the inclusion complex, a higher chitosan proportion led to the fastest release rate, while a higher alginate proportion resulted in the slowest. This study demonstrates that the form of curcumin incorporation and gel matrix composition critically influence the release profile. Our findings offer valuable insights for designing effective curcumin delivery systems, representing a significant advancement in biodegradable and sustainable drug delivery technologies.

Investigation of functionalized graphene oxide incorporated superabsorbent polymers for enhanced durability, hydration, microstructure and mechanical strength of modified concrete

ABSTRACT This study focuses on enhancing cementitious materials by incorporating silanized graphene oxide (SGO) and superabsorbent polymers (SAPs), aiming to improve their mechanical and durability properties. The primary goal is to evaluate the effects of SGO/SAP composites on the hydration, absorption, shrinkage, and overall performance of concrete. The composites were characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), thermogravimetric analysis (TGA), and transmission electron microscopy (TEM) to understand their microstructure. Mechanical and durability tests revealed that adding SGO/SAP composites significantly increased the mechanical strength and water absorption capabilities of the concrete. The compressive strength, split tensile strength, and flexural strength of the SGO/SAP-modified concrete were measured at 57 MPa, 4.90 MPa, and 8.25 MPa, respectively. Shrinkage tests demonstrated the composite hydrogel’s excellent water-holding capacity at 0.3 wt.% SGO/SAP, facilitating internal curing in concrete structures. FE-SEM analysis indicated a reduction in microcracks due to the presence of SGO/SAP. The improvements are attributed to the synergistic effects of SGO and SAP, which enhance water retention, dispersion, and interfacial bonding within the cementitious matrix. The microstructural studies confirmed the exceptional stability of the SGO/SAP-modified mix, emphasizing its potential as an additive to improve concrete properties. This research underscores the significant potential of SGO and SAP in advancing the performance of cement-based materials, highlighting their applicability in infrastructure development and construction for creating more durable and high-performing concrete structures.

Injectable Hydrogel With Glycyrrhizic Acid and Asiaticoside-Loaded Liposomes for Wound Healing.

Open skin wounds increase the risk of infections and can compromise health. Therefore, applying medications to promote healing at the injury site is crucial. In practice, direct drug delivery is often difficult to maintain for a long time due to rapid absorption or wiping off, which reduces the efficiency of wound healing. Consequently, the development of bioactive materials with both antibacterial and wound-healing properties is highly desirable. This study synthesized liposomes loaded with glycyrrhizic acid (GA) and asiaticoside (AS) by film dispersion-ultrasonication method, which were then incorporated into a GelMA solution and cross-linked by ultraviolet light to form a bioactive composite hydrogel for wound dressings. This hydrogel is conducive to the transport of nutrients and gas exchange. Compared with GelMA hydrogel (swelling rate 69.8% ± 5.7%), the swelling rate of GelMA/Lip@GA@AS is lower, at 52.1% ± 1.0%. GelMA/Lip@GA@AS also has better compression and rheological properties, and the invitro biodegradability is not significantly different from that of the collagenase-treated group. In addition, the hydrogel polymer has a stable drug release rate, good biocompatibility, and an angiogenic promoting effect. Invitro experiments prove that, at concentrations of 0.5, 1, 2, and 3 mg/mL, GelMA/Lip@GA@AS can inhibit the growth of Staphylococcus aureus. We synthesized GelMA/Lip@GA@AS hydrogel and found it possesses advantageous mechanical properties, rheology, and biodegradability. Experimental results invitro showed that the bioactive hydrogel could efficiently release drugs, exhibit biocompatibility, and enhance angiogenesis and antimicrobial effects. These results suggest the promising application of GelMA/Lip@GA@AS hydrogel in wound-dressing materials.

Investigation of the cushioning mechanism of a novel dental implant system with composite hydrogel

Background/purposeDental implants can restore both function and aesthetics in edentulous areas. However, the absence of cushioning mechanical behavior in implants may limit their clinical performance and reduce the long-term survival rates. This study aimed to establish an implant cushion mechanism that mimicked the natural periodontal ligament, utilizing the properties of composite hydrogels. Materials and methodsIn this study, we synthesized two composite hydrogels (HS and HSP groups) using hyaluronic acid (HA) and silk fibroin. We conducted static-constrained compression, creep, and porosity tests to assess the physical properties of these composite hydrogels. Finite element analysis (FEA) was employed to examine the effects of different thicknesses, permeabilities, and compression coefficients on the deformation of the hydrogels. The composite hydrogels were then applied within a novel dental implant, and the displacement performance of the implants, along with stress distribution on the alveolar bone, was evaluated using FEA. ResultsRegarding the mechanical performance of the composite hydrogels, increased permeability led to quicker displacement under compression. Thicker hydrogels with larger compression moduli influenced the biphasic behavior and deformation. The novel dental implants demonstrated biphasic sinking behavior under loading and rapid repositioning during unloading. When evaluating stress distribution on the alveolar bone under oblique loading, the HS and HSP implant groups showed a stress reduction of 10.3 % and 13.6 %, respectively, compared to commercial implant groups. ConclusionThis study highlights that the biphasic nature of solid and liquid phases is crucial when incorporating a cushioning mechanism into implants to replicate the characteristics of the periodontal ligament.

In-situ preparation of lanthanide luminescent MOF hydrogel for aldehyde detection☆

Metal-organic frameworks (MOFs) usually exist in the state of powder or crystal. When they are exposed to hydrophilic solvents, their structure will change and become unstable. Therefore, it is a challenge to construct MOF materials with tunable mechanical properties. Herein, we report in-situ growth lanthanide metal-organic framework (LnMOF) in sodium alginate (SA) and polyvinyl alcohol (PVA) hydrogel matrix. The prepared composite hydrogel not only displays characteristic lanthanide narrow-band emission under ultraviolet light, but also demonstrates excellent mechanical properties. The addition of LnMOF significantly enhances the compressive strength of the hydrogel (from 0.75 to 7.32 MPa). Furthermore, the composite hydrogel shows highly selective recognition of glutaraldehyde and gaseous formaldehyde at room temperature. The detection limits (LOD) of SP-EuMOF for glutaraldehyde and formaldehyde are 0.27 and 0.22 ppm, respectively. Based on these results, the LnMOF composite hydrogel is deemed to have significant potential as a fluorescent sensor for both glutaraldehyde and formaldehyde detection.

Drug loaded marine polysaccharides-based hydrogel dressings for treating skin burns.

Marine polysaccharide-based biomaterials possess a range of excellent functions and properties, such as antiviral, antioxidant, immune regulation, and promoting cell migration, and are widely used in modern medicine. In this study, a marine polysaccharide-based composite hydrogel was synthesized using carboxymethyl chitosan and oxidized fucoidan as matrix, and loads therapeutic drugs for the treatment of burn wounds infected with bacteria. The composite hydrogels can slowly release drugs at the wound site, providing a long-lasting therapeutic effect including antibacterial, antioxidant, and analgesic, in this way to facilitate the restoring of infected burn wounds by inhibiting bacterial infections, promoting cell migration, facilitating collagen regeneration, and restoring the abnormal alteration of factors such as IL-1β and CD86.

Structure regulation of oxidized soybean cellulose nanocrystals/poly-acrylamide hydrogel and its application potential in wound dressing

The development of functional dressings based on natural polysaccharide-based hydrogels remains a great challenge, and the specific roles of gel composition and drug-controlled release mechanisms were unclear. In this study, oxidized soybean cellulose nanocrystals (CNCs)/poly-acrylamide (PAM) hydrogel was prepared. The proportion of CNCs, crosslinkers, and water in the system was regulated to fine-tune the rheological performances, texture properties, transparency, and micro-network structures of CNCs/PAM hydrogel, and further explored its application potential in the field of wound dressings. It was found that CNCs improved the rigidity and adhesion of hydrogels, crosslinkers improved the network density, and water promoted the softening and fluidity of hydrogels. The effective filling of CNCs in the composite hydrogel was verified by FTIR, XRD, and NMR. Furthermore, the pH responsiveness and drug-loading potential of the smart hydrogel were tested by swelling and drug-controlled release experiments, elucidating drug-release dynamic mechanisms during the wound healing process. The inhibition zones (>7 mm) of gram-positive/negative bacteria and cell viability (>100 %) assay showed satisfactory biocompatibility, as the hydrogel effectively accelerated wound healing in a wound model. These results elucidated the regulation mechanism of the structures of CNCs/PAM hydrogel and revealed the application potential of CNCs/PAM hydrogel in wound dressings.

Porous chitosan quaternary ammonium salt hydrogel embedded with Cu, Ni and Pd nanoparticles for efficient coupled adsorption-catalytic reduction of methylene blue and 4-nitrophenol

Anthropogenic wastewater generation and water pollution can have negative impacts on public health and ecosystems. However, most materials do not have both adsorptive and catalytic properties, so the design and development of sustainable and multifunctional materials is essential for wastewater treatment. Herein, composite hydrogel (PHG) containing [2-(Methacryloyloxy)ethyl]dimethyl-(3-sulfopropyl) ammonium hydroxide (SBMA) and chitosan quaternary ammonium salts (HACC) were prepared for wastewater treatment. The adsorption capacities of the PHG hydrogels for nickel (NiII), copper (CuII), and palladium (PdII) ions were 158.68, 182.99, and 229.78 mg/g, respectively. The adsorption process is consistent with the Langmuir adsorption model and quasi-secondary kinetics. For further application of adsorbed metal ions, NaBH4 was selected for in situ reduction to prepare hydrogel-based catalysts cemented with metal nanoparticles (Ni-, Cu- and Pd-NPs), respectively. The PHG-Pd catalysts demonstrated significant catalytic efficiency in reducing 4-nitrophenol and methylene blue, and Kapp were 0.307 and 0.365 min−1, respectively. Among them, the activation parameters for the reduction of 4-NP over PHG-Pd catalyst were calculated as Ea = 36.27 kJ/mol, ΔH# = 33.72 kJ/mol and ΔS# = −259.68 J/(mol·K). This study is expected to provide insights into the design of multifunctional adsorption catalysts for the removal of dyes and nitro compounds from wastewater.

Injectable Oxygen-Carrying Microsphere Hydrogel for Dynamic Regulation of Redox Microenvironment of Wounds.

The delayed healing of infected wounds can be attributed to the increased production of reactive oxygen species (ROS) and consequent damages to vascellum and tissue, resulting in a hypoxic wound environment that further exacerbates inflammation. Current clinical treatments including hyperbaric oxygen therapy and antibiotic treatment fail to provide sustained oxygenation and drug-free resistance to infection. To propose a dynamic oxygen regulation strategy, this study develops a composite hydrogel with ROS-scavenging system and oxygen-releasing microspheres in the wound dressing. The hydrogel itself reduces cellular damage by removing ROS derived from immune cells. Simultaneously, the sustained release of oxygen from microspheres improves cell survival and migration in hypoxic environments, promoting angiogenesis and collagen regeneration. The combination of ROS scavenging and oxygenation enables the wound dressing to achieve drug-free anti-infection through activating immune modulation, inhibiting the secretion of pro-inflammatory cytokines interleukin-6, and promoting tissue regeneration in both acute and infected wounds of rat skins. Thus, the composite hydrogel dressing proposed in this work shows great potential for dynamic redox regulation of infected wounds and accelerates wound healing without drugs.

Stereolithography-assisted sodium alginate-collagen hydrogel scaffold with molded internal channels

Fabricating internal vascular networks within a hydrogel scaffold is essential for facilitating the supply of nutrients, oxygen, and metabolism exchange required by the encapsulated cells. The challenges in current hydrogel scaffold fabrication involve the difficulty of building adequate internal channels, poor scaffold geometry precision, and low cell viability caused by the fabrication process and polymer material properties. Stereolithography (SLA) stands out as a 3D printing technique distinguished by its superior production efficiency, advanced precision, and remarkable resolution in crafting intricate custom geometries. These attributes establish it as an innovative approach for templates in scaffold fabrication, potentially surpassing the fused deposition modeling (FDM)-based template strategy. Meanwhile, it exerts less shear stress on the cells compared to the direct bioprinting process. This novel strategy enables the fabrication of hydrogel vascular structure within the precision of 500 µm in both channel diameter and wall thickness. In this paper, various sodium alginate and collagen (SA-Col) composite hydrogels with varying collagen concentrations have been investigated to identify the optimal ratio for fabricating hydrogel scaffolds with channels.

An adhesive, highly stretchable and low-hysteresis alginate-based conductive hydrogel strain sensing system for motion capture

A strain sensor stands as an indispensable tool for capturing intricate motions in various applications, ranging from human motion monitoring to electronic skin and soft robotics. However, existing strain sensors still face difficulties in simultaneously achieving superior sensing performance sufficing for practical applications like high stretchability and low hysteresis, as well as seamless device fabrication like desirable interfacial adhesion and system-level integration. Herein, we develop a highly stretchable and low-hysteresis strain sensor with adhesive poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS)/polyacrylamide (PAAm)‑sodium alginate (SA) composite hydrogel, allowing the successful construction of a wireless motion capture sensing system that can provide precise data collection within a large deformation range. The resultant composite hydrogel displays favorable interfacial adhesion and robust mechanical stability, and the fabricated strain sensor demonstrates a wide working strain range (up to 500 %) with high sensitivity (gauge factor = 11) and ultra-low hysteresis (1.52 %), outperforming previous PEDOT-based hydrogel strain sensors. Enabled by the intriguing material properties and high sensing performance, we further demonstrate the fabrication and integration of a wireless motion capture sensing system for diverse applications like human motion monitoring, gesture recognition, and interactive communication.

Synthesis and Adsorption of Lead Ions by Chitosan–LDHs

Abstract With MgCl2 and AlCl3 as raw materials, nano Mg/Al LDHs were synthesized in situ during the process of chitosan gel formation, and then CS/LDHs composite multilayer hydrogels were prepared and characterized. After calcination at high temperature, they were used to adsorb Pb2+. The concentration of Pb2+ was measured using atomic absorption spectroscopy to investigate the adsorption performance of the composite material. The effects of pH value, initial concentration, and adsorption time on the adsorption efficiency were studied through single factor and orthogonal experiments. The results showed that the optimal process conditions for the adsorption of Pb2+ were pH=5, initial concentration of 2.5g/L, adsorption time of 30 minutes, removal rate of 70.65% at adsorption equilibrium, and adsorption capacity of 1150.32mg/g.

Locally Injectable Chitosan/β-Glycerophosphate Hydrogel Doped with Triptolide-Human Serum Albumin Nanoparticles for Treating Rheumatoid Arthritis.

Rheumatoid arthritis (RA) tends to occur in symmetrical joints and is always accompanied by synovial hyperplasia and cartilage damage. Triptolide (TP), an extract from Tripterygium, has anti-inflammatory and immunomodulatory properties and could be used in the treatment of RA. However, its poor water solubility and the multi-system lesions caused by the use of this substance limit its clinical application. Therefore, it would be of great significance to assemble a composite nanoparticle hydrogel and apply it to a collagen-induced arthritis (CIA) mouse model to investigate the therapeutic effect and biosafety of this compound. TP@HSA nanoparticles (TP@HSA NPs) were fabricated with a self-assembly method; a thermosensitive hydrogel loaded with the TP@HSA NPs (TP@HSA NP hydrogel) was prepared by using chitosan and beta- glycerophosphate (β-GP) and was then intra-articularly injected into CIA mice. The changes in joint swelling were measured with a digital caliper, and inflammation and cartilage damage were evaluated by using hematoxylin and eosin (H&E) and safranin O-fast green (SO&FG) staining, respectively. TP@HSA NPs with an average diameter of 112 ± 2 nm were successfully assembled, and their encapsulation efficiency and drug loading efficiency were 47.6 ± 1.5% and 10.6 ± 3.3%, respectively. The TP@HSA NP hydrogel had a gelation temperature of 30.5 ± 0.2 °C, which allows for its injection at low temperatures and its sol-gel transformation under physiological conditions within 2 min, making it a suitable drug depot. The TP@HSA NP hydrogel was intra-articularly injected into CIA mice; it released TP locally and exerted anti-inflammatory and immunomodulatory effects, alleviating synovial inflammation and cartilage damage effectively. We successfully fabricated a TP@HSA NP-loaded thermosensitive hydrogel with good biosafety, which can release TP slowly for the treatment of RA. Our study provides a basis for the development of TP-based innovative preparations and has good application prospects.

Temperature-responsive two-dimensional polydopamine hydrogel: Preparation, mechanisms, and applications in cancer treatment

Temperature-responsive hydrogels are advanced materials that exhibit significant physical or chemical changes in response to temperature variations. When the temperature reaches a specific threshold, these hydrogels alter their properties accordingly. They offer significant advantages in cancer therapy, including precise control over drug release, minimized toxicity, improved therapeutic efficacy, and biodegradability. Advancing the development of novel temperature-responsive hydrogels is crucial for enhancing therapeutic strategies. Herein, two-dimensional polydopamine (2D PDA) was first combined with chitosan (CTS) to create a temperature-responsive hydrogel for the control and release of anticancer drugs. Leveraging the carbonyl-rich nature of 2D PDA, we initiated a reversible cyclization reaction between CTS and the carbonyl groups on the surface of 2D PDA, resulting in a temperature-responsive CTS@2D PDA (CP) hydrogel. Furthermore, the CP hydrogel template was incorporated with the photosensitizer zinc phthalocyanine (ZnPc) and sodium percarbonate (SPC), an oxygen (O2) donor, to form a composite hydrogel (CSZP hydrogel). O2 released from the CSZP hydrogel mitigated solid tumor hypoxia and suppressed the expression of hypoxia-inducible factor-1α (HIF-1α), thereby augmenting the efficacy of photodynamic therapy (PDT). This temperature-responsive hydrogel represented a highly promising platform for the precise and controlled release of various therapeutics, thereby advancing the field of targeted disease treatment.

Bioinspired smart dual-layer hydrogels system with synchronous solar and thermal radiation modulation for energy-saving all-season temperature regulation

All-season thermal management with zero energy consumption and emissions is more crucial to global decarbonization over traditional energy-intensive cooling/heating systems. However, the static single thermal management for cooling or heating fails to self-regulate the temperature in dynamic seasonal temperature condition. Herein, inspired by the dual-temperature regulation function of the fur color changes on the backs and abdomens of penguins, a smart thermal management composite hydrogel (PNA@H-PM Gel) system was subtly created though an “on-demand” dual-layer structure design strategy. The PNA@H-PM Gel system features synchronous solar and thermal radiation modulation as well as tunable phase transition temperatures to meet the variable seasonal thermal requirements and energy-saving demands via self-adaptive radiative cooling and solar heating regulation. Furthermore, this system demonstrates superb modulations of both the solar reflectance (ΔR = 0.74) and thermal emissivity (ΔE = 0.52) in response to ambient temperature changes, highlighting efficient temperature regulation with average radiative cooling and solar heating effects of 9.6 °C in summer and 6.1 °C in winter, respectively. Moreover, compared to standard building baselines, the PNA@H-PM Gel presents a more substantial energy-saving cooling/heating potentials for energy-efficient buildings across various regions and climates. This novel solution, inspired by penguins in the real world, will offer a fresh approach for producing intelligent, energy-saving thermal management materials, and serve for temperature regulation under dynamic climate conditions and even throughout all seasons.