Al2O3 was deposited on silicon nanowire (SiNW) arrays by atomic layer deposition (ALD) as a passivation layer to reduce surface recombination velocity. As a result, effective minority carrier lifetime was improved from 1.82 to 26.2 μs. From this result, the relative low-surface recombination rate of 2.73 cm/s was obtained from a calculation using one-dimensional device simulation (PC1D). The performance of SiNW solar cells was also simulated by considering the surface recombination velocity on the side of SiNWs using two-dimensional device simulation. It was found that Al2O3 deposited by ALD can improve open-circuit voltage of SiNW solar cells even if the structure has a high-aspect ratio and large surface area. Therefore, improvement in the performance of SiNW solar cells can be expected.