Thin films of YBaCu(F)O were deposited on SrTiO3(100) substrates by multilayer deposition from three electron guns containing Y, BaF2, and Cu under a pressure of 5×10−5 Torr of O2. The films were later annealed in a separate chamber under a flowing O2‐H2O atmosphere. X‐ray diffraction studies reveal that the resulting structure is highly oriented with the a axis perpendicular to the substrate. Scanning electron micrographs show a morphology consisting of an array of orthogonal, interconnecting bars with well‐developed junctions. High‐resolution electron microscopy and electron diffraction patterns show that these junctions are atomically abrupt and that the associated c axes are mutually perpendicular. These epitaxial films show a sharp resistive transition with Tc(R=0) as high as 90 K. The zero field critical current density, determined from magnetization measurements, is 2.9×106 A/cm2 at 4.2 K and 5.0×104 A/cm2 at 77 K.