Hydrogels are promising starting materials for biomimetic soft robots as they are intrinsically soft and hold properties analogous to nature’s organic parts. However, the restrictive mold-casting and post-assembly fabrication alongside mechanical fragility impedes the development of hydrogel-based soft robots. Herein, we harness biocompatible alginate as a rheological modifier to manufacture 3D freeform architectures of both chemically and physically cross-linked hydrogels using the direct-ink-write (DIW) printing. The intrinsically hydrophilic polymer network of alginate allows the preservation of the targeted functions of the host hydrogels, accompanied by enhanced mechanical toughness. The integration of free structures and available functionalities from diversified hydrogel family renders an enriched design platform for bioinspired fluidic and stimulus-activated robotic prototypes from an artificial mobile tentacle, a bioengineered robotic heart with beating–transporting functions, and an artificial tendril with phototropic motion. The design strategy expands the capabilities of hydrogels in realizing geometrical versatility, mechanical tunability, and actuation complexity for biocompatible soft robots.

Fabrication of ultrathin 2D nonlayered nanomaterials remains challenging, yet significant due to the new promises in electrochemical functionalities. However, current strategies are largely restricted to intrinsically layered materials. Herein, a combinatorial self‐regulating acid etching and topotactic transformation strategy is developed to unprecedentedly prepare vertically stacked ultrathin 2D nonlayered nickel selenide nanosheets. Due to the inhibited hydrolyzation under acidic conditions, the self‐regulating acid etching results in ultrathin layered nickel hydroxides (two layers). The ultrathin structure allows limited epitaxial extension during selenization, i.e., the nondestructive topotactic transformation, enabling facile artificial engineering of hydroxide foundation frameworks into ultrathin nonlayered selenides. Consequently, the exquisite nonlayered nickel selenide affords high turnover frequencies, electrochemical surface areas, exchange current densities, and low Tafel slopes, as well as facilitating charge transfer toward both oxygen and hydrogen evolution reactions. Thus, the kinetically favorable bifunctional electrocatalyst delivers advanced and robust overall water splitting activities in alkaline intermediates. The integrated methodology may open up a new pathway for designing other highly active 2D nonlayered electrocatalysts.

Adaptive tendril coiling of climbing plants has long inspired the artificial soft microsystem for actuation and morphing. The current bionic research efforts on tendril coiling focus on either the preparation of materials with the coiling geometry or the design of self-shaping materials. However, the realization of two key functional features of the tendril, the spring-like buffering connection and the axial contraction, remains elusive. Herein, we devise a conductive tendril by fusing conductive yarns into tendril configuration, bypassing the prevailing conductivity constraints and mechanical limitations. The conductive tendril not only inherits an electrophysiology buffering mechanics with exceptional conductance retention ability against extreme stretching but also exhibits excellent contractive actuation performance. The integrative design of the ultraelastic conductive tendril shows a combination of compliant mobility, actuation, and sensory capabilities. Such smart biomimetic material holds great prospects in the fields of ultrastretchable electronics, artificial muscles, and wearable bioelectronic therapeutics.

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Pyroelectric materials are important functional materials that can generate an electrical response upon a temperature change. In recent years, significant advances have been achieved in different types of lead-free pyroelectrics and are rising to potential energy-related applications.