H. Paik:, :S. Xie:, H. Shin, C. Choi, J.H. Le, :C. Dong:, :J.A. Robinson (2DCC):, :J.-H. Lee:, J.-H. Ahn, G.Y. Yeom, :D.G. Schlom (PARADIM):, J. Kim (MIT):Project Summary::Remote epitaxy has drawn attention as it offers epitaxy of functional materials that can be released from the substrates with atomic precision, thus enabling production and heterointegration of flexible, transferrable, and stackable freestanding single-crystalline membranes. In this highlight, 2DCC and PARADIM team up to work with the inventor of remote epitaxy, Prof. Kim (MIT), to unveil the respective roles and impacts of the substrate material, graphene, substrate–graphene interface, and epitaxial material for electrostatic coupling of these materials, which governs cohesive ordering and can lead to single-crystal epitaxy in the overlying film.