The composition of atmospheric deposition is a measure of air quality, an important aspect of the health of the ecosystem. Consequently, continuous monitoring of atmospheric deposition is crucial to obtain remedial measures to avoid undesirable aspects that would affect living things. In this context, the objective of this study was to determine the rainwater quality at selected locations in Kandy and Peradeniya area of Sri Lanka, namely, Kandy city, Polgolla and University of Peradeniya (UOP), and to identify possible correlations between quality parameters through statistical means. Forty (40) rainwater samples from the UOP site and seven (07) samples each from the Kandy city and Polgolla sites were collected from the 18th May 2020 to 28th April 2021. The volume weighted average (VWA) pH values of UOP, Kandy and Polgolla sites were determined to be 7.44, 7.19 and 7.19, respectively, and moreover, acid rain (pH < 5.6) occurrences were not detected during the sampling period. The VWA values of rainfall, conductivity, salinity, TDS and hardness at the UOP site were 40.12 mm, 51.93 µS cm− 1, 0.0300 ppt, 26.59 mg L− 1 and 13.55 mg L− 1, respectively. The corresponding values of the Kandy city site were 16.52 mm, 64.04 µS cm− 1, 0.0361 ppt, 30.80 mg L− 1 and 19.49 mg L− 1, respectively; and those of the Polgolla site were 33.10 mm, 53.90 µS cm− 1, 0.0310 ppt, 25.76 mg L− 1 and 19.31 mg L− 1, respectively. The VWA values of conductivity, salinity, TDS were the highest at the Kandy city site. Further, the VWA values of hardness at Kandy and Polgolla were approximately equal, probably due to spring of Ca2+ and Mg2+ particulates from the dolomite quarry located in Digana area. The most prominent anion was identified as Cl− in bulk deposition at all three sites, while NO3− showed the lowest concentration of all sites. Moreover, very strong significant positive correlations were identified between conductivity-TDS, conductivity-salinity, conductivity-hardness, TDS-hardness, TDS-salinity, salinity-hardness, SO42− - Cl−, and NO3− - Cl− according to relevant Pearson correlation coefficients. It is thus concluded that the pollutants come from the same sources, either natural or anthropogenic.