The present study analyzes data from total suspended particulate (TSP) samples collected during 3 years (2005–2008) at Nainital, central Himalayas, India and analyzed for carbonaceous aerosols (organic carbon (OC) and elemental carbon (EC)) and inorganic species, focusing on the assessment of primary and secondary organic carbon contributions (POC, SOC, respectively) and on source apportionment by positive matrix factorization (PMF). An average TSP concentration of 69.6 ± 51.8 µg m−3 was found, exhibiting a pre-monsoon (March–May) maximum (92.9 ± 48.5 µg m−3) due to dust transport and forest fires and a monsoon (June–August) minimum due to atmospheric washout, while carbonaceous aerosols and inorganic species expressed a similar seasonality. The mean OC/EC ratio (8.0 ± 3.3) and the good correlations between OC, EC, and nss-K+ suggested that biomass burning (BB) was one of the major contributing factors to aerosols in Nainital. Using the EC tracer method, along with several approaches for the determination of the (OC/EC)pri ratio, the estimated SOC component accounted for ~25% (19.3–29.7%). Furthermore, TSP source apportionment via PMF allowed for a better understanding of the aerosol sources in the Central Himalayan region. The key aerosol sources over Nainital were BB (27%), secondary sulfate (20%), secondary nitrate (9%), mineral dust (34%), and long-range transported mixed marine aerosol (10%). The potential source contribution function (PSCF) and concentration weighted trajectory (CWT) analyses were also used to identify the probable regional source areas of resolved aerosol sources. The main source regions for aerosols in Nainital were the plains in northwest India and Pakistan, polluted cities like Delhi, the Thar Desert, and the Arabian Sea area. The outcomes of the present study are expected to elucidate the atmospheric chemistry, emission source origins, and transport pathways of aerosols over the central Himalayan region.