Layer transfer of BaTiO3 thin films onto silicon-based substrates has been investigated. Hydrogen and helium ions were co-implanted to facilitate ion-implantation-induced layer transfer of films from BaTiO3 single crystals. From thermodynamic equilibrium calculations, we suggest that the dominant species during cavity nucleation and growth are H2, H+, H2O, Ba2+ and Ba–OH, and that the addition of hydrogen to the Ba–Ti–O system can effectively suppress volatile oxide formation during layer transfer and subsequent annealing. After ion implantation, BaTiO3 layers contain microstructural defects and hydrogen precipitates in the lattice, but after layer transfer, the single crystal is found to be stoichiometric. Using direct wafer bonding and layer splitting, single crystal BaTiO3 thin films were transferred onto amorphous Si3N4 and Pt substrates. Micro-Raman spectroscopy indicated that the density of defects generated by ion implantation in BaTiO3 can be significantly reduced during post-transfer annealing, returning the transferred layer to its single crystal state. Characterization using piezoresponse force microscopy shows that the layer transferred thin films are ferroelectric, with domain structures and piezoresponse characteristics similar to that of bulk crystals.