This investigation determines ambient air arsenic (As), As(III), and As(V) concentrations in total suspended particulates (TSP) and dry deposition. Calculated/measured dry deposition flux ratios of ambient air As, As(III) and As(V) were evaluated using two dry deposition models at five characteristic sampling sites during 2009-2010.The highest average concentrations of As, As(III) and As(V) in TSP and dry deposition were measured at the Quan-xing industrial sampling site during AugustJanuary. The Quan-xing site, with many industrial factories under process around there regions, its air is extremely polluted. In addition, the average dry deposition velocities for ambient air total arsenic (As) at Bei-shi, Chang-hua, He-mei, Quanxing and Gao-mei were 0.60 (cm/sec), 0.57 (cm/sec), 0.73 (cm/sec), 0.67 (cm/sec) and 0.66 (cm/sec), respectively at these five characteristic sampling sites.The highest average seasonal variation for As, As(III) and As(V) in TSP and dry deposition were in winter and fall due to emissions from fossil fuel combustion by the nearby Taichung Thermal Power Plant (TTPP) and for household heating. The Noll and Fang model can be applied to predict dry deposition of As, As(III), and As(V) at these sampling sites.