LAUSR

Advanced optical materials with rational designs and tunable light transmission have been drawing increasing interest due to their great potential in energy‐efficient buildings and on‐demand optical devices. Mechanoresponsive smart windows (SWs) can modulate light transmittance by mechanical actuation, showing high energy efficiency, low cost, and chemical stability. However, current research mainly focuses on tensile strain‐responsive SWs that typically require a large strain to achieve optical transparency switching‐which causes great inconvenience to practical application and fatigue damage to matrix materials. Herein, a novel shear‐responsive SW with high strain sensitivity is fabricated by vertically fixing a Fe3O4@SiO2 nanochains (NCs) array in an elastic polyacrylamide matrix. The flexible SW exhibits optically transparent with all NCs standing vertically to the SW surface at initial relaxation state, which enables a good shielding effect, with NCs tilting along the shearing direction as the strain applied. Critically, a rather small shear displacement (1.5 mm) applied on the surface of SW gives rise to tunable optical states varying from the transparency state of 65% transmittance to the opaque state of 10%. The as‐prepared SW with novel tuning modulation, high shear strain sensitivity, and optical angle‐dependence holds promising potential in smart windows, optical switches, anti‐voyeurism, and etc.