Smart devices, such as soft robots, artificial organs, and soft actuators, require materials that adapt their morphologies and properties in response to their environment. These materials can be obtained through the composition of different types of materials that exhibit different responses to environmental stimuli, arranged in a rational spatial configuration. We achieved unique responsive materials by forming interfaces and surfaces of appropriate materials using the sol–gel method. In recent decades, we have proposed the use of wrinkles and nano-brushes on sol–gel-derived materials for various sophisticated applications, such as micropattern fabrication, wettability control, and linear actuators for size-selective transportation. This account introduces environment-responsive materials with rational interfaces via the sol–gel method, particularly those characterized by surface morphology.Graphical Materials with unique environmental responsiveness such as micropattern fabrication, wettability control, and linear actuating can be achieved by forming interfaces and surfaces using the sol–gel method.