Air pollution can be detected through rainwater composition. In this study, long-term measurements (2000-2014) of wet deposition were made to evaluate the physicochemical interaction and the potential sources of pollution due to changes of land use. The rainwater samples were obtained from an urban site in Kuala Lumpur and a highland-rural site in the middle of Peninsular Malaysia. The compositions of rainwater were obtained from the Malaysian Meteorological Department. The results showed that the urban site experienced more acidity in rainwater (avg=277mm, range of 13.8 to 841mm; pH=4.37) than the rural background site (avg=245mm, range of 2.90 to 598mm; pH=4.97) due to higher anthropogenic input of acid precursors. The enrichment factor (EF) analysis showed that at both sites, SO42-, Ca2+ and K+ were less sensitive to seawater but were greatly influenced by soil dust. NH4+ and Ca2+ can neutralise a larger fraction of the available acid ions in the rainwater at the urban and rural background sites. However, acidifying potential was dominant at urban site compared to rural site. Source-receptor relationship via positive matrix factorisation (PMF 5.0) revealed four similar major sources at both sites with a large variation of the contribution proportions. For urban, the major sources influence on the rainwater chemistry were in the order of secondary nitrates and sulfates>ammonium-rich/agricultural farming>soil components>marine sea salt and biomass burning, while at the background site the order was secondary nitrates and sulfates>marine sea salt and biomass burning=soil components>ammonia-rich/agricultural farming. The long-term trend showed that anthropogenic activities and land use changes have greatly altered the rainwater compositions in the urban environment while the seasonality strongly affected the contribution of sources in the background environment.