The electrical properties and field-emission characteristics of ZnO nanowires (ZnO-NWs) fabricated using a vapor-liquid-solid method were systematically investigated. In particular, we explored the effects of Al-doped ZnO (AZO) films (thickness 4-100 nm) deposited on ZnO-NWs using an atomic layer deposition (ALD) method on the optoelectronic properties. The results show that the sheet resistance of net-like ZnO-NW structures can be significantly improved, specifically to become ∼1/1000 of the sheet resistance of the as-grown ZnO-NWs, attaining less than 10 Ω Sq-1. The emission current density measured at the maximum field was roughly quadrupled relative to that of the as-grown ZnO-NWs. The data of the enhanced field-emission characteristics show that, with the ALD system, the AZO films of small resistance are readily coated on a structure with a high aspect ratio and the coating radius is controlled relative to the turn-on voltage and current density. The ultrathin AZO film from a one-monolayer coating process also significantly improved emission properties through modification of the effective work function at the AZO/ZnO-NW surface.