In this paper a novel buffer layer architecture consisting of LaMnO3/MgO/TiN is proposed as a suitable structural and chemical template for the epitaxial growth of high-transition temperature (Tc) superconductors on Cu metal surfaces. Using techniques such as high-energy electron diffraction and scanning transmission electron microscopy, we present in situ and ex situ analyses of the buffer-layer and superconductor growth with focus on structural properties of the interfaces formed. While MgO is a good barrier to oxygen diffusion, we find that MgO alone is not a suitable buffer layer due to rapid Cu diffusion. Further, growth of MgO with a single epitaxy can be hindered by the presence of impurities such as S, which form strongly bonded superstructures on the metal surface. With the addition of a TiN layer as a barrier to Cu diffusion, oxide formation is suppressed, interfaces are clean, and a single cube-on-cube epitaxy is observed. While the Cu/TiN and TiN/MgO interfaces are rough, the MgO and LaMnO3 layers planarize the material, leading to growth of smooth YBa2Cu3O7−δ (YBCO). Residual strain in the YBCO film is 0.25% or less and does not lead to apparent cracking. The superconducting properties of the samples were investigated by electrical transport and magnetization measurements. For the first time, high critical current density (Jc) values are reported for YBCO films grown on (001) single-crystal and 100‹100›?textured Cu surfaces without intervening metal coatings. Jc on single crystal-like substrates is as high as 3.5 MA/cm2. Reduced Jc of approximately 1 MA/cm2 on rolled Cu tapes is limited by damage to the tape surface during the rolling process.