Beside pigment absorption and reflection by periodic photonic structures, natural species often use light scattering to achieve whiteness. Synthetic hydrogels offer opportunities in stimuli‐responsive materials and devices; however, they are not conventionally considered as ideal materials to achieve high whiteness by scattering due to the ill‐defined porosities and the low refractive index contrast between the polymer and water. Herein, a poly( N ‐isopropylacrylamide) hydrogel network with percolated empty channels (ch‐PNIPAm) is demonstrated to possess switchable bright whiteness upon temperature changes, obtained by removing the physical agarose gel in a semi‐interpenetrating network of agarose and PNIPAm. The hydrogel is highly transparent at room temperature and becomes brightly white above 35 °C. Compared to conventional PNIPAm, the ch‐PNIPAm hydrogel exhibits 80% higher reflectance at 800 nm and 18 times faster phase transition kinetics. The nanoscopic channels in the ch‐PNIPAm facilitate water diffusion upon phase transition, thus enabling the formation of smaller pores and enhanced whiteness in the gel. Furthermore, fast photothermally triggered response down to tens of milliseconds can be achieved. This unique property of the ch‐PNIPAm hydrogel to efficiently scatter visible light can be potentially used for, e.g., smart windows, optical switches, and, as demonstrated in this report, thermoresponsive color displays.

Driving systems out of equilibrium under feedback control is characteristic for living systems, where homeostasis and dissipative signal transduction facilitate complex responses. This feature not only inspires dissipative dynamic functionalities in synthetic systems but also poses great challenges in designing novel pathways. Here we report feedback-controlled systems comprising two coupled hydrogels driven by constant light, where the system can be tuned to undergo stable homeostatic self-oscillations or damped steady states of temperature. We demonstrate that stable temperature oscillations can be utilized for dynamic colours and cargo transport, whereas damped steady states enable signal transduction pathways. Here mechanical triggers cause temperature changes that lead to responses such as bending motions inspired by the single-touch mechanoresponse in Mimosa pudica and the frequency-gated snapping motion inspired by the plant arithmetic in the Venus flytrap. The proposed concepts suggest generalizable feedback pathways for dissipative dynamic materials and interactive soft robotics.

The ability to switch adhesion strength is a highly desirable property for adhesives applied in a wet environment. The major challenges involve the presence of a water layer between the substrate and adhesive, and the incorporation of efficient switching mechanisms. Despite the recent progresses in devising such systems, there exist several intrinsic limitations in the current strategies, such as high residual adhesion, the use of solid–liquid transition, or thin film configurations. Herein, a channeled poly(N‐isopropylacrylamide) (PNIPAm) hydrogel containing bio‐inspired dopamine‐comonomers is reported, which undergoes temperature‐controlled reversible switching of underwater adhesion on both hydrophilic and hydrophobic surfaces. The introduction of microscopic channels inside the hydrogel, achieved by removing a sacrificial agarose network, greatly facilitates water removal from the interface and thus promotes underwater adhesive strength. On glass, the maximum adhesive stress of the channeled hydrogel can reach six times that of hydrogels without channels. Additionally, high switching efficiency and low residual adhesion can be achieved by the thermal phase transition of the PNIPAm network, also demonstrated by the capture and release of lightweight, irregular, fragile, and biological objects using the hydrogel. The channeling strategy provides implications for designing future underwater adhesive systems for, e.g., soft robotics or biomedical applications.