AbstractComposite films consisting of wrinkles on top of the elastomeric poly(dimethylsiloxane) film and a thin layer of silica particles embedded at the bottom is prepared as on‐demand mechanoresponsive smart windows. By carefully varying the wrinkle geometry, silica particle size, and stretching strain, different initial optical states and a large degree of optical transmittance change in the visible to near infrared range with a relatively small strain (as small as 10%) is achieved. The 10% pre‐strain sample has shallow wrinkles with a low amplitude and shows moderate transmittance (60.5%) initially and the highest transmittance of 86.4% at 550 nm when stretched at the pre‐strain level. Stretching beyond the pre‐strain level leads to a drastic decrease of the transmittance at 550 nm, 39.7% and 70.8% with an additional 10% and 30% strain, respectively. The large drop of optical transmittance is the result of combined effects from the formation of secondary wrinkles and nanovoids generated around the particles. The 20% pre‐strain sample has wrinkles with a moderate amplitude, showing 36.9% transmittance in the initial state, and the highest transmittance of 71.5% at 550 nm when stretched to the pre‐strain level. Further stretching leads to increased opacity similar to that seen from the 10% pre‐strain sample.