This study investigated the feasibility of monitoring arsenic (As) levels in total suspended particulates (TSP), in both dry deposition and dry deposition flux at five sampling sites located in central Taiwan during the years of 2009–2010. Experimental results indicate that the average As concentration in TSP and dry deposition was highest in Quan-xing (industrial) and lowest in Gao-mei (wetland). The mean As composition in TSP was highest in Hei-mei (residential) and lowest in Gao-mei (wetland). The average highest arsenic (As) of seasonal concentrations and compositions in TSP, dry deposition were occurred in winter and fall denotes that fossil fuel combustion by Taichung thermal power plant (TTPP) emissions and heating by household were the main reasons responsible for the high data values measured. Atmospheric concentrations of arsenic (As) were analyzed by a ICP-MS (Perkin Elmer Sciex ELAN DRC II). Finally, best-fit model can be used successfully in the prediction of ambient air pollutants around suburban/coastal, downtown, residential, industrial and wetland areas.