Cerium dioxide (CeO 2 ) cap layers for high temperature superconducting coated conductors were fabricated on yttria-stabilized zirconia (YSZ) single crystal substrates via the unbalanced radio frequency (RF) magnetron sputtering method. YBa 2 Cu 3 O 7− (YBCO) films were epitaxially deposited on the as-grown CeO 2 /YSZ (001) stacks using water-free metal organic deposition (MOD) method. The surface morphology evolution of CeO 2 cap layers could be tuned by adjusting the sputtering pressure, from smooth and uniformly granular, to rough and composed of spindle-like islands. According to the atomic force microscopy (AFM) data, a monotonic relationship could be found between the root mean squared (RMS) roughness value and flat area fraction. The critical current density (J c ) of the MOD-YBCO film varied significantly along with the CeO 2 morphology evolution, caused by the degradation of YBCO film's epitaxial growth. It was found that the as-grown CeO 2 cap layer deposited at 0.5 Pa could serve as a favorable template and did not require post-modification, on which YBCO film with J c of 1.92 MA/cm 2 (77 K, self-field) could be obtained. The MOD process would be improved in our future study by parameter optimization to enhance the J c property of YBCO films.