High‐performance multifunctional nanocoatings not only protect and enhance substrate materials, but also offer additional functionalities. This demands a sophisticated coordination of the coating's inherent properties and microstructural features. Here we present a multi‐functional active nanocoating via meta‐structural engineering of covalent organic framework (COF) deposition materials. Our COF nanocoating, characterized by well‐defined micropores (1‐2 nm), meta‐structured textures (30‐300 nm), tailored thickness (100‐300 nm), and good uniformness, showcases a unique combination of angle‐independent structural coloration and ultrafast responsiveness to gaseous stimuli. Remarkably, it demonstrates good compatibility with a wide range of inert substrate materials, from rigid ones like glass and metal to flexible elastomers and nanomaterial films of various shapes and sizes. This versatility enables the facile development of devices that can optically report information about their environments. Examples include chemically active coatings with ultrafast (∼ 10 ms) color‐changing behaviors and programmable actuation behaviors upon exposure to gaseous stimuli, and mechanically active coatings that can detect substrate strain up to 50% yet maintain structural robustness and consistent coloration hue. We believe that meta‐structural engineering of COF nanocoatings on inert substrates could enable them to respond to environmental stimuli, potentially indicating a new trend in developing multifunctional materials and smart devices.This article is protected by copyright. All rights reserved