Polymer nanocomposites exhibiting remarkable mechanical properties are a focus of research for decades in structural applications. However, their practical application faces challenges due to poor interfacial load transfer, nanofiller dispersion, and processing limitations. These issues are critical in achieving stiff, strong, lightweight, and structurally integrated materials. Additionally, they often suffer from predetermined properties, which may not be effective under specific loading conditions. Addressing these challenges, the development of design strategies for mechano‐responsive materials has advanced, enabling self‐adaptive properties that respond to various mechanical stimuli. Drawing inspiration from natural systems, these approaches have been implemented in synthetic material systems, leveraging the design flexibility of nanocomposites as needed. Key focus areas include exploring mechanoradical reactions for dynamic mechano‐responsiveness, as well as utilizing biomimetic mineralization and mechanical training for self‐strengthening. This work also examines multistability, enabling on‐demand deformation of materials and structures. Recent advancements in viscoelastic damping and nonreciprocal materials are discussed, highlighting their potential for directional energy absorption, transmission, and vibration control. Despite the need for significant improvements for real‐world applications, mechano‐responsive polymers and nanocomposites are expected to offer enormous opportunities not only in structural applications but also in other fields such as biomedical engineering, energy harvesting, and soft robotics.