including the use of liquid crystals, [7] suspended particles, [8] photonic crystals, [9] and chromogenic materials driven by temperature, [10] light, [11] mechanical force, [6,12] magnetic field, [13] and electrical field. [14] However, it still faces great challenges in practical uses of the smart optical materials, especially in smart windows, for example, due to the complicated process, high cost, and low efficiency for the preparation and fabrication of such smart windows. Therefore, it is highly desirable to develop simple and effective strategies to design new smart optical materials with rapid responsive time, large transmittance modulation, and good repeatability, which may open up new opportunities for applications in large-area smart windows.Wrinkling (or buckling) is a ubiquitous phenomenon that occurs in both natural [15] and artificial systems, [12a,16] with dimensions across a wide range of length scale from meters down to nanometers. Artificial wrinkles can be generated by introducing compressive stresses to a skin layer/elastomer substrate bilayer film through various approaches, such as thermal stress, [17] mechanical stress, [18] capillary force, [19] light-driven photoisomerization, [20] and osmotic pressure. [21] Owing to their spontaneous nature, versatility, and tunability or even total reversibility in response to external stimuli, surface wrinkling has provided an effective platform to create smart, controllable, and responsive surface topography and subsequently to dynamically tune functionality, which inspired various important applications including flexible electronic devices, [22] tunable diffraction gratings, [23] microlens arrays, [24] dry adhesives, [25] dynamic scaffolds, [26] and optical devices. [27] Since mechanical force as an external stimuli has many advantages such as simple and independent control of the amount, direction, and timing of strain, [28] some recent studies have demonstrated that mechanoresponsive surface wrinkles offer an effective and repeatable strategy to dynamically tune optical properties on-demand by changing the surface topography in responsive to mechanical force. For example, the light transmittance of mechanoresponsive surface wrinkles for smart windows has been dynamically tuned by means of micro-and nanopillar arrays on wrinkled elastomers, [28,29] harnessing Preparation of surface wrinkles on a skin layer/elastomer substrate bilayer film has attracted extensive attention because of their unique and broad applications in flexible electronic devices, tunable diffraction gratings, and smart windows. However, it still remains a great challenge to develop a general strategy for fabricating mechanoresponsive surface wrinkles using various skin layer materials with wide tunability of wrinkles' wavelength and amplitude, large optical modulation range, rapid optical switching rate, and high stability. Here, a general, simple, and cost-effective strategy is reported, through uniaxially stretching and subsequently releasing skin layer/elastomer substrate...