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Abstract The primary mechanism of optical memoristive devices relies on phase transitions between amorphous and crystalline states. The slow or energy‐hungry amorphous–crystalline transitions in optical phase‐change materials are detrimental to the scalability and performance of devices. Leveraging an integrated photonic platform, nonvolatile and reversible switching between two layered structures of indium selenide (In₂Se₃) triggered by a single nanosecond pulse is demonstrated. The high‐resolution pair distribution function reveals the detailed atomistic transition pathways between the layered structures. With interlayer “shear glide” and isosymmetric phase transition, switching between the α‐ and β‐structural states contains low re‐configurational entropy, allowing reversible switching between layered structures. Broadband refractive index contrast, optical transparency, and volumetric effect in the crystalline–crystalline phase transition are experimentally characterized in molecular‐beam‐epitaxy‐grown thin films and compared to ab initio calculations. The nonlinear resonator transmission spectra measure of incremental linear loss rate of 3.3 GHz, introduced by a 1.5 µm‐long In₂Se₃‐covered layer, resulted from the combinations of material absorption and scattering.