High throughput, low‐temperature deposition, sharp interfaces, and selective deposition with direct ion‐, electron‐, and photon‐beam‐controlled techniques are some of the key driving forces for the development of superconducting thin films by metalorganic chemical vapor deposition (MOCVD) technique. In this paper we report on the electrical and structural properties of Y‐Ba‐Cu‐O (YBCO) films deposited by MOCVD on yttrium‐stabilized zirconia (YSZ) and BaF2/YSZ substrates using a single‐stepinsituprocessing method which requires no further annealing. YBCO films deposited on BaF2/YSZ substrates have zero resistance at 80 K. The films were characterized by energy dispersive x‐ray analysis, x‐ray diffraction, scanning electron microscopy, and transmission electron microscopy. The films on BaF2/YSZ substrates exhibited textured growth having both thecandaaxis perpendicular to the substrate. The use of BaF2as a buffer layer suggests three‐dimensional integration of high‐temperature superconducting thin film for hybrid superconductor/semiconductor devices as well as superconductor switches and other related devices.