Variable Stiffness Actuators with Covalently Attached Nanofragments that Induce Mineralization

Abstract Soft robotics has attracted great attention owing to their immense potential especially in human–robot interfaces. However, the compliant property of soft robotics alone, without stiff elements, restricts their applications under load‐bearing conditions. Herein, biohybrid soft actuators, that create their own bone‐like rigid layer and thus alter their stiffness from soft to hard, are designed. Fabrication of the actuators is based on polydimethylsiloxane (PDMS) with an Au film to make a soft substrate onto which polypyrrole (PPy) doped with poly(4‐styrenesulfonic‐co‐maleic acid) sodium salt (PSA) is electropolymerized. The PDMS/Au/PPy(PSA) actuator is then functionalized, chemically and physically, with plasma membrane nanofragments (PMNFs) that induce bone formation within 3 days, without using cells. The resulting stiffness change decreases the actuator displacement; yet a thin stiff layer cannot completely stop the actuator's movement, while a relatively thick segment can, but results in partial delamination the actuator. To overcome the delamination, an additional rough Au layer is electroplated to improve the adhesion of the PPy onto the substrate. Finally, an alginate gel functionalized with PMNFs is used to create a thicker mineral layer mimicking the collagen‐apatite bone structure, which completely suppresses the actuator movement without causing any structural damage.