Recently, the plasma electrolytic oxidation (PEO) process has been widely studied and applied in the industrial setting due to its ability to create functional oxide layers on Al, Ti, Mg, and Zr alloys. In this work, a pulsed direct current (DC) power supply was adopted to grow the zirconia coating on pure Zr metal by PEO treatment. A fixed frequency of 1000 Hz and constant current of 2 A were used to fabricate all zirconia coatings. Duty cycle values of 25%, 75%, and 100% were used and 0.1 M K3PO4 aqueous solution containing three different concentrations of KOH, 0.01, 0.05 and 0.1 M, was also used in fabrication. The plasma breakdown voltage decreased with increasing KOH concentration due to its higher electrolyte conductivity. The PEO oxide coating consisted of a thin continuous barrier layer and a thick porous outermost layer, which consisted of mainly monoclinic and minor tetragonal ZrO2 phases. The PEO treatment of Zr metal provided excellent corrosion resistance in Hank's solution and good biocompatibility for 3T3 and MG63 cells. These results suggest that PEO coatings having potential applications in the biomedical field were confirmed in this study.