Additional Crosslinking Research Articles

Modeling the Maturation of the Vocal Fold Lamina Propria Using a Bioorthogonally Tunable Hydrogel Platform.

Toward the goal of establishing an engineered model of the vocal fold lamina propria (LP), mesenchymal stem cells (MSCs) are encapsulated in hyaluronic acid (HA)-based hydrogels employing tetrazine ligation with strained alkenes. To mimic matrix stiffening during LP maturation, diffusion-controlled interfacial bioorthogonal crosslinking is carried out on the soft cellular construct using HA modified with a ferocious dienophile, trans-cyclooctene (TCO). Cultures are maintained in MSC growth media for 14 days to afford a model of a newborn LP that is homogeneously soft (nLP), a homogeneously stiffened construct zero (sLP0) or 7 days (sLP7) post cell encapsulation, and a mature LP model (mLP) with a stiff top layer and a soft bottom layer. Installation of additional HA crosslinks restrictscell spreading. Compared to the nLP controls, sLP7 conditions upregulate the expression of fibrous matrix proteins (Col I, DCN, and FN EDA), classic fibroblastic markers (TNC, FAP, and FSP1), and matrix remodeling enzymes (MMP2, TIMP1, and HAS3). Day 7 stiffening also upregulates the catabolic activities, enhances ECM turnover, and promotes YAP expression. Overall, in situ delayed matrix stiffening promotes a fibroblast transition from MSCs and enhances YAP-regulated mechanosensing.

Chemical and structural induced ductile-to-brittle transition in electrospun silica nanofiber membranes

Electrospun silica nanofiber membranes show a high potential in many advanced environmental applications. However, little is known about their mechanical performance which could be a limiting factor for further innovation. It is shown in this work that silica nanofiber membranes have a completely different deformation behavior compared to conventional polymeric/thermoplastic nanofiber membranes, resulting from their significant differences in chemical and physical properties such as fiber interactions and porosity. Furthermore, storage at room temperature initiates remarkable changes in failure mechanisms, depending on the storage humidity, which can be accelerated via a thermal treatment. These changes are linked to the structural changes of the membrane resulting from its chemical reactivity towards moisture in the air. Additional interactions and crosslinks are observed, leading to fiber shrinkage and rearrangement. As a result, more contact points are created between nanofibers, creating additional friction forces and, as such, a complete shift in mechanical properties towards a stronger, stiffer, and more brittle material (tensile strength of 14.0 ± 3.8 MPa vs. 3.1 ± 0.4 MPa and failure strain of 0.9 ± 0.2% vs. 24.2 ± 1.0%). The silica nanofiber membranes thus allow mechanical tunability via altering the storage or treatment conditions.

3D printing of concentrated nanocellulose material: The critical role of substrates on the shape fidelity and mechanical properties

This paper presents a breakthrough in the shape fidelity and mechanical strength of 3D-printed high-concentration nanocellulose structures, demonstrating a record flexural strength of 149 ± 2 MPa and a flexural modulus of 15 ± 0.8 GPa. These findings replace the previous method of 3D printing on conventional substrates with wood substrates for highly concentrated nanocellulose (HCNC) structures. The HCNC structures are 3D-printed using extrusion and processed under controlled drying conditions (Relative humidity: 60 % and 45 %, Temperature: 25 °C) to achieve outstanding mechanical properties without sacrificing structure shape fidelity/retention. It was noticed that the drying phenomenon of HCNC structures on the conventional substrates is responsible for the adhesion issues between the printed layers resulting in low shape fidelity/retention. In contrast with conventional substrates, the wood substrates offer an increased drying rate from the bottom side of printed HCNC structures due to its hydrophilicity and wicked nature, which helps maintain the shape fidelity without using additional crosslinkers, resulting in improved shape fidelity/retention and mechanical properties. The 3D-printed nanocellulose structure bears twice the load compared to a commercial poly lactic acid 3D-printed one. These features open a new horizon for fabricating 3D-printed nanocellulose structures for advanced environmentally friendly structural applications.

Synthesis of copolymer nanocomposite by in situ intercalative polymerization for batch and fixed bed adsorption

AbstractPartially neutralized acrylic acid (AA)/sodium acrylate (NaAA) and N, N′‐methylenebisacrylamide (MBA) were subjected to intercalative copolymerization in aqueous solution of polyvinyl alcohol (PVA) in the presence of sodium montmorillonite (NaMMT) nano clay to prepare filled semi‐interpenetrating network (FSIPN) type composite polymer networks. Filled Full IPN (FFIPN) composites were prepared in a similar way by additional crosslinking of PVA with maleic acid (MA) crosslinker. The polymers were characterized with FTIR, NMR, XRD, TGA, SEM, EDAX, TEM, XPS, DLS, PZC, and pH reversibility test. The synthesis variables were optimized with respect to batch adsorption of 100 mg/L each of methyl violet (MV) and congo red (CR) dye as response using the central composite design (CCD) of response surface methodology (RSM). The FFIPN prepared from polyacrylic acid (PAA)/sodium polyacrylate containing PVA/Clay/MBA/MA of optimized composition of 4/1.5/0.75/4 (wt.% of AA/NaAA), respectively, showed an optimized adsorption (mg/g adsorbent) of 459.16/417.31 of MV/CR as single dye and 438.01/417.31 of MV/CR in 1:1 binary mixtures of 100 mg/L feed concentration. The FFIPN showed an adsorption (mg/g) of 41.54/37.61 and removal% of 88.5/80.12 at a feed flow rate, bed height, and feed inlet concentration of 20 mL/min, 20 mm, and 50 mg/L, respectively.

Self-crosslinked alkaline polyelectrolyte membranes with exceptional stability under dry-wet alternating conditions

The emergence of alkaline polyelectrolytes (APEs) with high stability and high ionic conductivity has greatly improved the power density of alkaline polyelectrolyte fuel cells (APEFCs), now the cell stability has become an urgent problem to be addressed. The uneven distribution of humidity and hydration state inside large-scale electrodes will cause the membrane to swell and shrink repeatedly, resulting in the membrane rupture and/or the peeling off of catalyst layers, which is a fatal problem affecting the stability of APEFCs. In the present work, we report a new APE, self-crosslinked quaternary ammonia poly (N-methyl-piperidine-terphenyl and 7-bromo-tri-fluoro-heptanone), denoted as xQAPTF. The crosslinking network inside the membrane can be formed without introducing additional crosslinking agents, and can effectively limit the membrane swelling degree in water (only 4% at 80oC). More importantly, the xQAPTF membranes exhibit excellent mechanical strength and flexibility even after multiple all-wet-all-dry cycles. Under the dry-wet alternating condition (RH repeatedly switched between 100% and 50%), the APEFC using xQAPTF membrane run stably, with the cell voltage switching accordingly and steadily. Such a unique quality of APE membranes has so far not been reported in the literature, which strongly enhances the practicality of APEs, as well as the APEFC and relevant technologies.

Engineering multicomponent tissue by spontaneous adhesion of myogenic and adipogenic microtissues cultured with customized scaffolds

The integration of intramuscular fat—or marbling—into cultured meat will be critical for meat texture, mouthfeel, flavor, and thus consumer appeal. However, culturing muscle tissue with marbling is challenging since myocytes and adipocytes have different media and scaffold requirements for optimal growth and differentiation. Here, we present an approach to engineer multicomponent tissue using myogenic and adipogenic microtissues. The key innovation in our approach is the engineering of myogenic and adipogenic microtissues using scaffolds with customized physical properties; we use these microtissues as building blocks that spontaneously adhere to produce multicomponent tissue, or marbled cultured meat. Myocytes are grown and differentiated on gelatin nanofiber scaffolds with aligned topology that mimic the aligned structure of skeletal muscle and promotes the formation of myotubes in both primary rabbit skeletal muscle and murine C2C12 cells. Pre-adipocytes are cultured and differentiated on edible gelatin microbead scaffolds, which are customized to have a physiologically-relevant stiffness, and promote lipid accumulation in both primary rabbit and murine 3T3-L1 pre-adipocytes. After harvesting and stacking the individual myogenic and adipogenic microtissues, we find that the resultant multicomponent tissues adhere into intact structures within 6–12 h in culture. The resultant multicomponent 3D tissue constructs show behavior of a solid material with a Young’s modulus of ∼ 2 ± 0.4 kPa and an ultimate tensile strength of ∼ 23 ± 7 kPa without the use of additional crosslinkers. Using this approach, we generate marbled cultured meat with ∼ mm to ∼ cm thickness, which has a protein content of ∼ 4 ± 2 g/100 g that is comparable to a conventionally produced Wagyu steak with a protein content of ∼ 9 ± 4 g/100 g. We show the translatability of this layer-by-layer assembly approach for microtissues across primary rabbit cells, murine cell lines, as well as for gelatin and plant-based scaffolds, which demonstrates a strategy to generate edible marbled meats derived from different species and scaffold materials.

All-natural and high-performance structural material based on lignin-reinforced cellulose

Sustainable materials derived from lignocellulosic resources are attractive alternatives to ubiquitous petrochemical plastics. However, it remains a huge challenge to improve the mechanical properties of lignocellulosic materials through efficient and low-energy processing strategy. Herein, we report a facile lignin-reinforced cellulose strategy to manufacture an all-natural and high-performance structural material from bamboo particles via partial delignification followed by hot-pressing. Partial delignification can regulate the amount of lignin in the bamboo particles and release internal cellulose microfibers. The subsequent hot-pressing drives residual lignin into the cellulose matrix to form a dense structure, which acts as a polyphenolic binder to improve the performance of the structural material. The obtained lignin-reinforced cellulose plate (LRCP) demonstrates high isotropic flexural strength (∼162 MPa), which is higher than that of natural bamboo and typical petrochemical plastics. Moreover, LRCP shows outstanding toughness (∼2.58 MPa m1/2), excellent compressive strength (∼178 MPa), improved wet stability and superior flame resistance. LRCP is all-natural and eco-friendly without the need for additional chemical cross-linking reagents. We believe that this facile and cost-effective strategy provides a promising way to process lignocellulosic resources into all-natural and high-performance structural materials that can serve as powerful plastic alternatives in the future.

Metal ions-assisted construction of SiO2/MXene/Fe3O4 aerogel as multifunctional electromagnetic wave absorbing material

Advanced electromagnetic wave absorbing materials are developing towards the directions of lightweight, thin thickness, broad absorption bandwidth, and multifunction. MXene, as a new type of two-dimensional material, has received widespread attention, but it is necessary to address the impedance mismatch problem caused by its high conductivity. In this work, Fe3O4/MXene composite aerogel is prepared by metal ion-assisted crosslinking method without adding additional crosslinking agents. And a layer of hydrophobic fumed silica is further sprayed on the aerogel. Benefiting from the magneto-electric synergistic effect and the porous structure, SiO2/MXene/Fe3O4 aerogels shows excellent electromagnetic wave absorption performances, achieving a quite broad absorption bandwidth up to 8.8 GHz at an extremely thin thickness of 1 mm. The hybrid aerogel also shows superhydrophobic and thermal insulation properties, which are conducive to improving the resistance to harsh environments and thus endow the absorbers with a long service time.

3D printing of mechanically functional meniscal tissue equivalents using high concentration extracellular matrix inks

Decellularized extracellular matrix (dECM) has emerged as a promising biomaterial in the fields of tissue engineering and regenerative medicine due to its ability to provide specific biochemical and biophysical cues supportive of the regeneration of diverse tissue types. Such biomaterials have also been used to produce tissue-specific inks and bioinks for 3D printing applications. However, a major limitation associated with the use of such dECM materials is their poor mechanical properties, which limits their use in load-bearing applications such as meniscus regeneration. In this study, native porcine menisci were solubilized and decellularized using different methods to produce highly concentrated dECM inks of differing biochemical content and printability. All dECM inks displayed shear thinning and thixotropic properties, with increased viscosity and improved printability observed at higher pH levels, enabling the 3D printing of anatomically defined meniscal implants. With additional crosslinking of the dECM inks following thermal gelation at pH 11, it was possible to fabricate highly elastic meniscal tissue equivalents with compressive mechanical properties similar to the native tissue. These improved mechanical properties at higher pH correlated with the development of a denser network of smaller diameter collagen fibers. These constructs also displayed repeatable loading and unloading curves when subjected to long-term cyclic compression tests. Moreover, the printing of dECM inks at the appropriate pH promoted a preferential alignment of the collagen fibers. Altogether, these findings demonstrate the potential of 3D printing of highly concentrated meniscus dECM inks to produce mechanically functional and biocompatible implants for meniscal tissue regeneration. This approach could be applied to a wide variety of different biological tissues, enabling the 3D printing of tissue mimics with diverse applications from tissue engineering to surgical planning.

Dynamic Metal-Ligand Coordination-Assisted Ionogels for Deformable Alternating Current Electroluminescent Devices.

Overcoming the trade-off between the mechanical robustness and conductivity of ionic conductors is a crucial challenge for deformable ionotronics. In this work, we propose a simple but effective gelation strategy for selectively improving the mechanical robustness of ionogels without compromising their ionic conductivity. To achieve this, we introduce dynamic metal-ligand coordination chemistry into the ionic liquid (IL)-insoluble domains of a physically crosslinked ionogel network structure. As a result, the overall mechanical property is remarkably improved with the aid of additional chemical crosslinking. This strategy does not require any additional heat/light (UV) treatments to induce chemical crosslinking. The homogeneous physically/chemically dual crosslinked ionogel films can be readily obtained by simply casting a solution containing Ni2+ sources, copolymer gelators, and ILs. The effects of adjusting fundamental parameters on the ionogel properties are investigated systematically. The optimized mechanically robust and highly conductive ionogels are successfully employed as deformable ionic electrodes in alternating-current electroluminescent displays, indicating their high practicality. Overall, these results validate that exploiting metal-ligand coordination dynamic bonding is an extremely straightforward strategy for selectively improving the mechanical characteristics of conductive ionogels, which are promising platforms for deformable ionotronics.

A Liquid Metal Microdroplets Initialized Hemicellulose Composite for 3D Printing Anode Host in Zn-Ion Battery.

Maintaining a steady affinity between gallium-based liquid metals (LM) and polymer binders, particularly under continuous mechanical deformation, such as extrusion-based 3D printing or plating/stripping of Zinc ion (Zn2+ ), is very challenging. Here, an LM-initialized polyacrylamide-hemicellulose/EGaIn microdroplets hydrogel is used as a multifunctional ink to 3D-print self-standing scaffolds and anode hosts for Zn-ion batteries. The LM microdroplets initiate acrylamide polymerization without additional initiators and cross-linkers, forming a double-covalent hydrogen-bonded network. The hydrogel acts as a framework for stress dissipation, enabling recovery from structural damage due to the cyclic plating/stripping of Zn2+ . The LM-microdroplet-initialized polymerization with hemicellulosescan facilitate the production of 3D printable inks for energy storage devices.

Harnessing plum (Prunus domestica L.) processing wastes for the fabrication of bio-composite edible films: An attempt towards a food circular bioeconomy

This study investigated the effects of different biopolymer matrices on the quality characteristics of edible films produced from plum kernel protein isolate (PKPI), arrowroot starch (ARS), and plum kernel oil (PKO). All eight film-forming matrices produced a self-supporting and peelable film. Among the formulations tested, a composite film containing 50% PKPI, 50% ARS, and 1% PKO (P50S50O) exhibited favourable features, including the highest glass transition temperature and tensile strength, which were 2.05 and 1.59-folds higher than PKPI film, respectively. The composite film (P50S50O) showed a reduced water vapour transmission rate (WVTR), permeance, and water vapour permeability (WVP) indicating a decreased affinity for moisture and an improved tortuosity of the vapour diffusion path. XRD analysis revealed a 55.75% increase in crystallinity, and SEM micrographs showed smoother and more homogeneously entrapped PKO in P50S50O films. Peak shifting in FT-IR spectra confirmed the development of additional cross-linking among various film-forming matrices, which improved the barrier, mechanical, and thermal properties of the composite films, paving the way for the prospective application of plum processing waste in the development of edible films and curbing the environmental pollution of plastics films.

An injectable and self-healing hydrogel with dual physical crosslinking for in-situ bone formation.

Although hydrogels have been widely studied because of their satisfactory biocompatibility and plasticity, their application is limited in bone tissue engineering (BTE) owing to their inadequate mechanical properties and absence of osteogenic activity. To address this issue, we developed an updated alendronate (ALN)-Ca2+/Mg2+-doped supramolecular (CMS) hydrogel based on our previously developed mechanically resilient "host-guest macromer" (HGM) hydrogel to improve the hydrogel's mechanical properties and osteogenic activity. The CMS hydrogel was prepared by introducing a new physical crosslinking comprising the strong chelation of the comonomer acrylate alendronate (Ac-ALN) and Ca2+/Mg2+ in the HGM hydrogel. Compared with the previously developed HGM hydrogel, the upgraded CMS hydrogel presented better mechanical properties because of the additional physical crosslinking, while possessing injectable and self-healing properties like the HGM hydrogel. Moreover, the addition of Ac-ALN and Ca2+/Mg2+ also effectively promoted the in vitro proliferation, migration, and osteogenic differentiation of bone marrow-derived stem cells. The healing effect of a rat cranial defect further proved that the in vivo bone regeneration ability of CMS hydrogel was better than that of HGM hydrogel. The updated CMS hydrogel shows significant potential for BTE application.

A novel strategy inspired by steaming Chinese steamed bread for preparation of tannin-furanic rigid bio-foam

Tannin-furanic rigid foam material has been receiving extensive attention due to its renewable, easy-preparation, lightweight, thermal insulation, and flame retardancy, that been considering a potential flame-retardants and thermally-insulating materials in construction field. The most fashionable approaches for tannin-furanic foam manufacturing, currently, are the self-blowing expansion with the aid of blowing agent with/without extra heating, and foaming via mechanical stirring in presence of non-environmentally friendly crosslinker. Herein, a novel and green strategy was proposed for tannin-furanic rigid foam preparation without blowing agent and additional crosslinker by steam-driven foaming. The performance of steam-driven tannin-furanic based foam (SDTF) was evaluated systematically and a possible foaming mechanism was suggested. The results indicated that a totally different surface but similar microstructure morphology of SDTF was developed, which displayed a larger cell size and thicker cell wall than standard tannin-furanic-formaldehyde foam (STF). A much lower pulverization ratio (approximately 4.6%) was reached for SDTF with respect to STF even though its compression strength was only less than half. An excellent thermal insulation performance was verified by the thermal conductivity of SDTF, only approximately 0.0286 W/m·K, which is considered ultra-low value that the STF cannot reach or seldom reach after STF modification or/and special structure design. The flame retardancy of SDTF was investigated by LOI and ignition experiment, which demonstrated a strong flame resistance and self-extinguishing nature, rendering it superior to STF. This preparation strategy provides a promising sustainable and environmentally friendly method for fabrication of green tannin-furanic foam for industry applications.

A facile strategy and mechanism to achieve biobased bismaleimide resins with high thermal-resistance and strength through copolymerizing with unique propargyl ether-functionalized allyl compound

Preparing biobased thermosetting resins with high mechanical properties and superior heat resistance is an important issue for the sustainable development and applications of high performance resins. Herein, a novel biobased allyl compound (DBB) with aryl propargyl ether groups was synthesized from renewable honokiol, which was then used to copolymerize with 4,4′-bismaleimidodiphenylmethane (BDM) to develop new biobased resins (BDM/DBB). The effects of the molar ratio of BDM to DBB on the thermal and mechanical properties were studied. Results show that all BDM/DBB resins possess both high thermal and mechanical properties. Specifically, their glass transition temperatures (Tg > 440 °C) and storage moduli (> 1.3 GPa at 400 °C) are higher than those of biobased allyl compounds modified BDM resins reported so far (SCI database); moreover, their initial thermal decomposition temperatures are about 448 °C and flexural strengths range from 106 to 117 MPa. These excellent comprehensive performances are attributed to the unique crosslinked network resulted from the complex curing mechanism of BDM/DBB, which including the copolymerization between imide groups and allyl groups as well as the additional thermal crosslinking of aryl propargyl ether. This work provides a sustainable and facile strategy to construct high performance biobased resins.

Thermo‐Responsive Nanocomposite Bioink with Growth‐Factor Holding and its Application to Bone Regeneration (Small 9/2023)

Thermo-Responsive Nanocomposite Bioinks Poly(organophosphazene)-based thermo-responsive nanocomposite bioink, with tunable mechanical property under a moderate temperature range, exhibits good 3D printing outcomes without additional chemical crosslinking process. The bioink encapsulates growth factors through physical interaction, exhibiting biological activities and therapeutic potential for bone defect repair. More details can be found in article number 2203464 by Soo-Chang Song and co-workers.

Post‐curing and structural relaxation of epoxy networks during early stages of aging for civil engineering applications

AbstractIn this work, epoxy networks used for civil engineering constructions are aged at ambient temperature, and the impact of the early stages of aging on mechanical properties is analyzed. It is observed that Young's modulus and the yield stress increase with the aging time whereas the strain at break and the toughness decrease. The structural causes for these variations are investigated by swelling experiments, infrared spectroscopy, thermogravimetric analysis, differential scanning calorimetry, and dynamic mechanical analysis. By combining experimental results, it is deduced that the aging process occurs in two stages. During the first 7 days of aging, the change in mechanical properties should essentially be attributed to the postcuring, which results in additional crosslinking reactions. When increasing the aging time to 21 days, the crosslinking density reaches a plateau, but a second stage emerges, in which the mechanical properties continue evolving in the same way, with variations of the mechanical parameters being of comparable amplitude. This second stage is attributed to the evolution of the thermodynamic state of the glass, leading to a densification of the epoxy network through minimization of the free volume, and favoring the creation of physical interactions between polymer segments. Therefore, structural relaxation is shown to have a significant impact on the mechanical properties.

Chemically Fueled Dissipative Cross-Linking of Protein Hydrogels Mediated by Protein Unfolding.

Cells assemble dynamic protein-based nanostructures far from equilibrium, such as microtubules, in a process referred to as dissipative assembly. Synthetic analogues have utilized chemical fuels and reaction networks to form transient hydrogels and molecular assemblies from small molecule or synthetic polymer building blocks. Here, we demonstrate dissipative cross-linking of transient protein hydrogels using a redox cycle, which exhibit protein unfolding-dependent lifetimes and mechanical properties. Fast oxidation of cysteine groups on bovine serum albumin by hydrogen peroxide, the chemical fuel, formed transient hydrogels with disulfide bond cross-links that degraded over hours by a slow reductive back reaction. Interestingly, despite increased cross-linking, the hydrogel lifetime decreased as a function of increasing denaturant concentration. Experiments showed that the solvent-accessible cysteine concentration increased with increasing denaturant concentration due to unfolding of secondary structures. The increased cysteine concentration consumed more fuel, which led to less direction oxidation of the reducing agent and affected a shorter hydrogel lifetime. Increased hydrogel stiffness, disulfide cross-linking density, and decreased oxidation of redox-sensitive fluorescent probes at a high denaturant concentration provided evidence supporting the unveiling of additional cysteine cross-linking sites and more rapid consumption of hydrogen peroxide at higher denaturant concentrations. Taken together, the results indicate that the protein secondary structure mediated the transient hydrogel lifetime and mechanical properties by mediating the redox reactions, a feature unique to biomacromolecules that exhibit a higher order structure. While prior works have focused on the effects of the fuel concentration on dissipative assembly of non-biological molecules, this work demonstrates that the protein structure, even in nearly fully denatured proteins, can exert similar control over reaction kinetics, lifetime, and resulting mechanical properties of transient hydrogels.

Nanocellulose-Based Biomaterial Ink Hydrogel for Uptake/Release of Bovine Serum Albumin

This study explores the potential of using nanocellulose extracted from oil palm empty fruit bunch (OPEFB) as a biomaterial ink for 3D printing. The research focuses on using nanocellulose hydrogels for the controlled uptake and release of proteins, with the specific protein solution being Bovine Serum Albumin (BSA). To provide a suitable material for the bioprinting process, the study examines the characteristics and properties of the printed hydrogels through various analyses, such as morphology, functional group, crystallinity, and compression test. Several parameters, such as initial concentration, temperature, and the presence of calcium chloride as an additional crosslinker, affect the protein uptake and release capabilities of the hydrogel. The study is important for biomedicine as it explores the behavior of protein uptake and release using nanocellulose and 3D printing and can serve as a preliminary study for using hydrogels in biological materials or living cells.

Visible light-responsive nanocomposite g-C3N4/CNC/PAM aerogel constructed through in-situ photoinitiation for management of wastewater containing organic/heavy metal compound contaminants

Facing the increasingly serious water pollution problem, photocatalytic method has been recognized as one of the best solutions due to its convenience, efficiency and low consumption. Graphitic carbon nitride (g-C3N4), a metal-free and visible light-responsive photocatalyst, has shown great potential in the photocatalytic treatment of water pollution. This study describes a novel bottom-up strategy for constructing visible light-responsive photoactive nanocomposite g-C3N4/CNC/PAM aerogel with the g-C3N4 uniformly loaded throughout a polymeric network, perfect mechanical property and high performance in treating wastewater containing organic/heavy metal compound contaminants. Aldehyde-modified negatively charged natural nanoparticle cellulose nanocrystal (CNC-CHO) was used to achieve uniform dispersion of g-C3N4, and also participate in the subsequent formation of aerogel through chemical crosslinking with photoinitiated polyacrylamide (PAM) catalyzed by g-C3N4 without additional crosslinkers. The optimized porous structure of the prepared aerogel ensured high swelling rate of up to 2500%, excellent pollutant adsorption performance and high light transmittance, thus achieved high removal rate and removal efficiency for different types of pollutants including organic dyes (RhB, MB and CR) and heavy metal Cr(VI). The removal efficiency could get 99% for RhB (5 mg/L) in 6 h, and 95% for Cr (VI) (10 mg/L) in 100 min under visible light. Further more, the aerogel showed excellent mechanical stability and reusability, with no loss in activity observed after over 5 cycles of dye degradation.