Abstract
Plant tissues are constructed as composite material systems of stiff cellulose microfibers reinforcing a soft matrix. Thus, they comprise smart and multifunctional structures that can change shape in response to external stimuli due to asymmetrical fiber alignment and possess robust mechanical properties. Herein, we demonstrate the biomimetics of the plant material system using silk fiber-reinforced alginate hydrogel matrix biocomposites. We fabricate single and bilamellar biocomposites with different fiber orientations. The mechanical behavior of the biocomposites is nonlinear, with large deformations, as in plant tissues. In general, the bilamellar system shows increased modulus, strain UTS, and toughness compared to the single-lamellar system for most of the tested orientations. Overall, the biocomposites present a wide range of elastic modulus values (3.0 ± 0.6-104.7 ± 11.3 MPa) and UTS values (0.23 ± 0.04-12.5 ± 2.0 MPa). The bilamellar biocomposites demonstrated shape-transforming abilities with diverse morphing modes, emulating different plant tissues and creating complex shape-morphing structures. These multifunctional biocomposites possess tunable and robust mechanical properties, controllable shape-morphing deformations, and the ability to self-controlled encapsulation, grip, and release objects. By harnessing biomimetic principles, these soft, smart, and multifunctional materials hold potential applications spanning from soft robotics, medicine, and tissue engineering to sensing and drug delivery.