Adaptive functional materials which exhibit responses to external stimuli, such as temperature, humidity, pH, and light, have been a topic of interest towards applications of sensing, drug delivery, and actuation. In the present study, novel stimuli-responsive microstructures were designed on the surfaces of hybrid bilayered films, and their structural features, as a function of external stimuli, were closely investigated. PNIPAM/ hybrid silica and silica/PDMS bilayered films were demonstrated to exhibit thermal and solvent response, allowing the appearance/disappearance of the surface textures (wrinkles and folding). Moreover, the surface wrinkles and foldings were successfully formed on spherical core-shell particles. The morphological features of wrinkles on a spherical surface depends on curvature of the sphere, which is in good agreement with a previously-reported theoretical description. As an application, catch & release of micro-particles has been demonstrated.