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The realization of high-contrast modulation in optically transparent media is of great significance for emerging mechano-responsive smart windows. However, no study has provided fundamental strategies for maximizing light scattering during mechanical deformations. Here, a new type of 3D nanocomposite film consisting of an ultrathin (≈60 nm) Al2O3 nanoshell inserted between the elastomers in a periodic 3D nanonetwork is proposed. Regardless of the stretching direction, numerous light-scattering nanogaps (corresponding to the porosity of up