ZnO nanowires (NWs) with different radii (rNW) have been aligned between pre-patterned electrodes using dielectrophoresis (DEP) for the fabrication of high gain UV sensors. The DEP conditions (voltage amplitude and frequency) and electrode material, geometry and size were optimized to enhance the efficiency during the DEP process. To understand the alignment mechanism of the ZnO NWs, the dielectrophoretic force (FDEP) was analyzed as a function of the DEP conditions and NW dimensions. These studies showed that the DEP alignment process tends to trap NWs with a smaller radius. The effects of NW size on device performance were analyzed by means of I-V measurements in darkness and under illumination (200 nm < λ < 600 nm). In darkness, the NW resistance increases as rNW decreases due to the reduction of the conduction volume, until saturation is reached for rNW < 65 nm. On the other hand, the NW spectral photoresponse shows high values around 10(8) A W(-1) (measured at 5 V and λ < 370 nm) and follows a linear trend as a function of the NW cross section. In addition, the cut-off wavelength depends on rNW, presenting a clear blue-shift for NWs with a lower radius (rNW < 50 nm). Transient photoresponse studies show that NWs with lower radii have longer rise times and shorter decay times mainly due to surface trapping effects. Regardless of NW size, passivation of the surface using a dielectric capping layer of SiO2 reduces the dynamic range of the photoresponse due to a strong increase of the dark current.