In-plane anisotropy (IPA) due to asymmetry in lattice structures provides an additional parameter for the precise tuning of characteristic polarization-dependent properties in two-dimensional (2D) materials, but the narrow range within which such method can modulate properties hinders significant development of related devices. Herein we present a novel periodic phase engineering strategy that can remarkably enhance the intrinsic IPA obtainable from minor variations in asymmetric structures. By introducing alternant monoclinic and rutile phases in 2D VO2 single crystals through the regulation of interfacial thermal strain, the IPA in electrical conductivity can be reversibly modulated in a range spanning two orders of magnitude, reaching an unprecedented IPA of 113. Such an intriguing local phase engineering in 2D materials can be well depicted and predicted by a theoretical model consisting of phase transformation, thermal expansion, and friction force at the interface, creating a framework applicable to other 2D materials. Ultimately, the considerable adjustability and reversibility of the presented strategy provide opportunities for future polarization-dependent photoelectric and optoelectronic devices.
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