A specially designed combined process of pre-oxidation and nanofiltration membrane was utilized to remove As(III) in the contaminated water without reagent addition and sediment creation in this work. Different parameters that affected the rejections of As(III) and As(V) were discussed, including the initial concentration, pH of the feed, and the cross-flow filtration pressure. The rejection of As(III) was over 70% which was restricted to the high initial feed concentration, while it was around 40% under the other conditions. Whereas, the rejection of As(V) maintained above 95% in all tests. As a result, As(III) was first pre-oxidized before membrane filtration. The ozone and aeration oxidation methods were used to oxidize As(III). The effects of aeration time and oxidation time were studied. The experimental results indicated that the rejection of As(III) was increased to over 90% after pre-oxidation, and the permeate could meet the drinking water standard for As in China. Particularly, the aeration took a much longer oxidation time than ozone, but it was still a more suitable method as the pre-oxidation process because of its safety and easy operability.