Here, the recent progress of high-pressure research toward 2D materials and heterostructures, involving graphene, boron nitride, transition metal dichalcogenides, 2D perovskites, black phosphorene, MXene, and covalent–organic frameworks, using diamond anvil cell is summarized. This enables an insightful understanding of the variable vdW interaction induced structural changes, structure–property relations as well as contributes to the versatile implications of 2D materials. Pressure is an effective and clean tool that allows modifications of the electronic structure, crystal structure, morphologies, and compositions of 2D materials through van der Waals (vdW) interaction engineering. 2D materials possess wide-tuning properties ranging from semiconducting and metallization to superconducting, etc., which are determined by their structure, empowering them to be appealing in optoelectronic and photovoltaic applications.
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