Programmable Multi‐Responsive Nanocellulose‐Based Hydrogels With Embodied Logic

Abstract Programmable materials are desirable for a variety of functional applications that range from biomedical devices, actuators and soft robots to adaptive surfaces and deployable structures. However, current smart materials are often designed to respond to single stimuli (like temperature, humidity, or light). Here, a novel multi‐stimuli‐responsive composite is fabricated using direct ink writing (DIW) to enable programmability in both space and time and computation of logic operations. The composite hydrogels consist of double‐network matrices of poly( N ‐isopropylacrylamide) (PNIPAM) or poly(acrylic acid) (PAA) and sodium alginate (SA) and are reinforced by a high content of cellulose nanocrystals (CNC) (14 wt%) and nanofibers (CNF) (1 wt%). These composites exhibit a simultaneously tunable response to external stimuli, such as temperature, pH, and ion concentration, enabling precise control over their swelling and shrinking behavior, shape, and mechanical properties over time. Bilayer hydrogel actuators are designed to display bidirectional bending in response to various stimuli scenarios. Finally, to leverage the multi‐responsiveness and programmability of this new composite, Boolean algebra concepts are used to design and execute NOT, YES, OR, and AND logic gates, paving the way for self‐actuating materials with embodied logic.