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Van der Waals (vdW) epitaxial growth provides an efficient strategy to prepare heterostructures with atomically and electronically sharp interfaces. Herein, PbI2 was in situ thermally deposited onto exfoliated thin−layered CrOCl nanoflakes in high vacuum to fabricate vdW PbI2/CrOCl heterostructures. Optical microscopy, atomic force microscopy, X−ray diffraction, and temperature−dependent Raman spectroscopy were used to investigate the structural properties and phonon behaviors of the heterostructures. The morphology of PbI2 films on the CrOCl substrate obviously depended on the substrate temperature, changing from hemispherical granules to 2D nanoflakes with flat top surfaces. In addition, anomalous blueshift of the Ag1 and Au2 modes as the temperature increased in PbI2/CrOCl heterostructure was observed for the first time. Our results provide a novel material platform for the vdW heterostructure and a possible method for optimizing heterostructure growth behaviors.