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Inspired by the intriguing adaptivity of natural life, such as squids and flowers, we propose a series of dynamic and responsive multifunctional devices based on multiscale structural design, which contain metal nanocoating layers overlaid with other micro-/nanoscale soft or rigid layers. Since the optical/photothermal properties of a metal nanocoating are thickness dependent, metal nanocoatings with different thicknesses were chosen to integrate with other structural design elements to achieve dynamic multistimuli responses. The resultant devices demonstrate 1) strain-regulated cracked and/or wrinkled topography with tunable light-scattering properties, 2) moisture/photothermal-responsive structural color coupled with wrinkled surface, and 3) mechanically controllable light-shielding properties attributed to the strain-dependent crack width of the nanocoating. These devices can adapt external stimuli, such as mechanical strain, moisture, light, and/or heat, into corresponding changes of optical signals, such as transparency, reflectance, and/or coloration. Therefore, these devices can be applied as multistimuli-responsive encryption devices, smart windows, moisture/photothermal-responsive dynamic optics, and smartphone app–assisted pressure-mapping sensors. All the devices exhibit high reversibility and rapid responsiveness. Thus, this hybrid system containing ultrathin metal nanocoatings holds a unique design flexibility and adaptivity and is promising for developing next-generation multifunctional devices with widespread application.

A versatile wrinkle‐based micropatterned system with a film‐substrate structure is proposed, which contains a hydrophilic film of polyvinyl alcohol or its composite with laponite and a hydrophobic substrate of polydimethylsiloxane or its composite with carbon black. The wrinkled system features high design flexibility and multistimuli responsiveness, which can be activated by various mechanical methods, including vertical press or scratch, gentle stretch‐and‐release, bend, or analogous magneto‐mechanical and electro‐mechanical modes. The resultant wrinkles possess 1) instantaneous and reversible strain/moisture/light responsive optical modulation; 2) tunable dynamics for the aforementioned strain/moisture/light response;3) tailorable amplitude/wavelength; 4) unique surface morphologies from the coupling of wrinkles and cracks; 5) excellent reversibility and durability. A variety of applications are demonstrated based on this system, including 1) a moisture erasable highly sensitive pressure responsive device and pattern replicator with a high fidelity; 2) a moisture erasable scratch/magneto‐mechanical re‐writable tablet; 3) an electro‐mechanical controllable smart window with an ultra‐sensitive strain responsive transmittance modulation and a low operating voltage; 4) various types of strain responsive, moisture erasable, and laser writable information recording/encryption devices. This work provides new routes for designing innovative wrinkled systems triggered by diverse mechanical fashions and can decode multiple environmental stimuli into optical signals for widespread application.

The design of a dynamic, versatile, convertible, and responsive micropatterned system is realized by a photo/moisture reconstructible multiscale film‐substrate bilayer structure. Specifically, a hydrophilic polyvinyl alcohol (PVA)/laponite (LP) thin film is covalently bonded to a photothermally active polydimethylsiloxane (PDMS)/carbon black (CB) soft substrate. A laser engraver can inscribe programmable aligned micro‐wrinkles by manipulating laser power and spatiotemporal control. These wrinkles can be modulated into three distinct systems 1) moisture erasable and laser re‐writable wrinkles; 2) moisture driven reversible wrinkles; 3) moisture resistant wrinkles, which are achieved by controlling a) the moisture resistance of PVA; b) the dimensional stability of PVA/LP film regulated by the LP nanostructure, which can be adjusted by the laser power and the LP ratio. This programmable system can be applied in information encryption/recording and as a moisture responsive electrical switch, offering new routes for the modulations and applications of next generation smart materials.