Interfacial delamination processes for physically separating a film structure from a substrate, and processes of fabricating a thin-film electronic device. The processes entail providing the substrate with an electrically-conductive separation layer on a surface of the substrate and optionally providing a pin hole free barrier layer on the electrically-conductive separation layer, forming a film structure on the electrically-conductive separation layer or, if present, the barrier layer, to yield a multilayer structure, and separating the film structure from the substrate by subjecting the multilayer structure to interfacial debonding that comprises contacting at least an interface between the film structure and the electrically-conductive separation layer or, if present, the barrier layer, with water or an electrolyte solution.