We developed a successive ion layer adsorption and reaction method based on spin-coating (spin-SILAR) and applied the method to the fabrication of highly uniform ZnO/CdS core/shell nanowire arrays. Because the adsorption, reaction, and rinsing steps occur simultaneously during spin-coating, the spin-SILAR method does not require rinsing steps between the alternating ion adsorption steps, making the growth process simpler and faster than conventional SILAR methods based on dip-coating (dip-SILAR). The ZnO/CdS core/shell nanowire arrays prepared by spin-SILAR had a denser and more uniform structure than those prepared by dip-SILAR, resulting in the higher power efficiency for use in photoelectrochemical cells.