Synergizing Structural Stiffness Regulation with Compliance Contact Stiffness: Bioinspired Soft Stimuli‐Responsive Materials Design for Soft Machines

Stiffness regulation strategies endow soft machines with stronger functionality to cope with diverse application requirements, for example manipulating heavy items by improving structural stiffness. However, most programmable stiffness strategies usually struggle to preserve the inherent compliant interaction capabilities following an enhancement in structural stiffness. In this study, inspired by the musculocutaneous system, we propose a soft stimuli‐responsive material (SRM) by combining shape memory alloy into compliant materials. By characterizing the mechanical performance, the flexural modulus increases from 6.6 to 142.4 MPa under the action of active stimuli, crossing two orders of magnitude, while Young's modulus stays at 2.2 MPa during programming structural stiffness. This comparative result indicates that our SRMs can keep a lower contact stiffness for compliant interaction although structural stiffness increases. Then, we develop three diverse soft machines to show the application potential of this smart material, such as robotic grippers, wearable devices, and deployable mechanisms. By applying our materials, these machines possess stronger load‐bearing capabilities. Meanwhile, these demonstrations also illustrate the efficacy of this paradigm in regulating the structural stiffness of soft machines while maintaining their compliant interaction capabilities.