Conducting polymer hydrogels (CPHs) have emerged as a fascinating class of smart soft matters important for various advanced applications. However, achieving the synergistic characteristics of conductivity, self-healing ability, biocompatibility, viscoelasticity, and high mechanical performance still remains a critical challenge. Here, we develop for the first time a type of multifunctional hybrid CPHs based on a viscoelastic polyvinyl alcohol (PVA)-borax (PB) gel matrix and nanostructured CNFs-PPy (cellulose nanofibers-polypyrrole) complexes that synergizes the biotemplate role of CNFs and the conductive nature of PPy. The CNF-PPy complexes are synthesized through in situ oxidative polymerization of pyrrole on the surface of CNF templates, which are further well-dispersed into the PB matrix to synthesize homogeneous CNF-PPy/PB hybrid hydrogels. The CNF-PPy complexes not only tangle with PVA chains though hydrogen bonds, but also form reversibly cross-linked complexes with borate ions. The multi-complexation between each component leads to the formation of a hierarchical three-dimensional network. The CNF-PPy/PB-3 hydrogel prepared by 2.0 wt % of PVA, 0.4 wt % of borax, and CNF-PPy complexes with a mass ratio of 3.75/1 exhibits the highest viscoelasticity and mechanical strength. Because of a combined reinforcing and conductive network inside the hydrogel, its maximum storage modulus (∼0.1 MPa) and nominal compression stress (∼22 MPa) are 60 and 2240 times higher than those of pure CNF/PB hydrogel, respectively. The CNF-PPy/PB-3 electrode with a conductivity of 3.65 ± 0.08 S m has a maximum specific capacitance of 236.9 F g, and its specific capacitance degradation is less than 14% after 1500 cycles. The CNF-PPy/PB hybrid hydrogels also demonstrate attractive characteristics, including high water content (∼94%), low density (∼1.2 g cm), excellent biocompatibility, plasticity, pH sensitivity, and rapid self-healing ability without additional external stimuli. Taken together, the combination of such unique properties endows the newly developed CPHs with potential applications in flexible bioelectronics and provides a practical platform to design multifunctional smart soft materials.

This article highlights the properties of stimuli-responsive bio-based polymeric systems and their main intelligent applications.

The rapid development of modern industry and excessive consumption of petroleum‐based polymers have triggered a double crisis presenting a shortage of nonrenewable resources and environmental pollution. However, this has provided an opportunity to stimulate researchers to harness native biobased materials for novel advanced materials and applications. Nanocellulose‐based aerogels, using abundant and sustainable cellulose as raw material, present a third‐generation of aerogels that combine traditional aerogels with high porosity and large specific surface area, as well as the excellent properties of cellulose itself. Currently, nanocellulose aerogels provide a highly attention‐catching platform for a wide range of functional applications in various fields, e.g., adsorption, separation, energy storage, thermal insulation, electromagnetic interference shielding, and biomedical applications. Here, the preparation methods, modification strategies, composite fabrications, and further applications of nanocellulose aerogels are summarized, with additional discussions regarding the prospects and potential challenges in future development.

Polydopamine (PDA), as the most typical kind of synthetic melanins, possesses similar interesting properties, such as antioxidation, photoprotection, metal chelation, and energy dissipation. During the past a few years, PDA...