In this review a strategy for the desing of bioinspired, smart, multiscale interfacial (BSMI) materials is presented and put into context with recent progress in the field of BSMI materials spanning natural to artificial to reversibly stimuli-sensitive interfaces. BSMI materials that respond to single/dual/multiple external stimuli, e.g., light, pH, electrical fields, and so on, can switch reversibly between two entirely opposite properties. This article utilizes hydrophobicity and hydrophilicity as an example to demonstrate the feasibility of the desing strategy, which may also be extended to other properties, for example, conductor/insulator, p-type/n-type semiconductor, or ferromagnetism/anti-ferromagnetism, for the design of other BSMI materials in the future.