In this study, Yttria-stabilized zirconia (YSZ) functional layers were applied with different thin-film fabrication process such as sputtering and atomic layer deposition (ALD) to enhance oxygen reduction reaction (ORR) for solid oxide fuel cells. We confirmed that the YSZ functional layer deposited with sputtering showed relatively low grain boundary density, while the YSZ functional layer deposited with the ALD technique clearly indicated high grain boundary density through scanning electron microscopy (SEM) and X-ray diffractometry (XRD) results. The YSZ functional layer coated with the ALD technique revealed that more ORR kinetics can occur using high grain boundary density than the functional layer deposited with sputtering. The peak power density of the SOFC deposited with ALD YSZ indicates 2-folds enhancement than the pristine SOFC.