Samples of Total Suspended Particulates (TSP) were collected at Pashan, Pune (semi-urban) and Sinhagad (rural) locations in India, during the winter season of 2003/4, using a high volume air sampler and were analyzed for major water-soluble chemical components using Ion Chromatograph and Atomic Absorption Spectrophotometer. Results of the study were compared with those reported for the same locations in winter season, about two decades back. It was observed that TSP and all of its chemical components showed marked increase in concentrations after the period of two decades at both Pune and Sinhagad. Especially, for NH4+, SO42-, NO3- and Ca2+, the concentrations increased by about 9, 7,7 and 4 times at Pune and about 23,10,10 and 6 times at Sinhagad, respectively. This feature shows the significant impact of anthropogenic activities at both the locations. SO42- is still the main acidifying component of aerosols and NH4+ dominates over Ca2+ in the neutralization of acidity in 2003/4 whereas earlier two decades back, Ca2+ was the major neutralizer.