to prepare, and some of them are chemically unstable during optical switching. [11] Furthermore, the assembly of these smart windows often suffers from complicated processes, high cost, and low efficiency. [1,3] Therefore, a convenient, cheap, and highly effective method is desirable for the fabrication of large-area smart windows with advanced functional features, such as large transmittance modulation, fast response time, and chemical stability suitable for long-term use without deteriorating optical performance.Micro-and nanostructured soft surfaces offer a new strategy to dynamically tune optical properties by changing the surface topography without affecting the bulk properties. [12][13][14][15][16][17][18][19] Recently, surface wrinkling [20][21][22] has become a very cost-effective, facile technology to reversibly control the surface topography, which inspired a wide range of applications such as thinfilm properties measurement, [23] tunable adhesion and wettability, [24] stretchable electronics, [25][26][27][28] and optical materials/ devices. [29][30][31][32][33][34][35][36][37][38] Some more recently studies have demonstrated that surface wrinkling can also be used to prepare large-area smart windows capable of controlling the light transmittance by means of micro-and nanopillar arrays on wrinkled elastomers, [12,13] crumpling of metallic nanofilms, [14] graphene films, [15] and graphene oxide films [16] on elastomeric substrates and silica nanoparticle-embedded elastomer composite. [17] It should be made clear that the light transmittance change mentioned in these studies is actually normal transmittance change, which was usually achieved by scattering the light rather than absorbing the light. Despite the clear advantages in material fabrication and stability, these methods still suffer from complicated fabrication processes, high cost, small transmittance modulation range, or potential material degradation. For example, smart windows achieved by micro-and nanopillar arrays on wrinkled elastomers [12,13] usually require multistep fabrication processes including template preparation, replica modeling, and surface wrinkling. Furthermore, these pillar arrays cannot be completely eliminated during the mechanical actuation which limits the achievable transmittance modulation range. For thin film/elastomer systems, [14][15][16] extremely large and more complicated biaxial prestrains (e.g., 400% for graphene oxide film/silicone rubber system [16] ) are usually required to realize very large surface topography change to enable large optical transmittance tuning. And also, the thin film materials are Optical devices with tunable specular optical transmittance have recently attracted great interest due to their wide range of applications. However, the reported methods of realizing tunable optical transmittance suffer from complex fabrication processes, high cost, unstable materials, or low tuning range. In this study, a simple, cheap, and highly effective approach to achieve large tuning range of optical transm...