The development of infrastructure, a rapidly increasing population, and urbanization has resulted in increasing air pollution levels in the African city of Addis Ababa. Prior investigations into air pollution have not yet sufficiently addressed the sources of atmospheric particulate matter. This study aims to identify the major sources of fine particulate matter (PM2.5) and its seasonal contribution in Addis Ababa, Ethiopia. Twenty-four-hour average PM2.5 mass samples were collected every 6th day, from November 2015 through November 2016. Chemical species were measured in samples and source apportionment was conducted using a chemical mass balance (CMB) receptor model that uses particle-phase organic tracer concentrations to estimate source contributions to PM2.5 organic carbon (OC) and the overall PM2.5 mass. Vehicular sources (28%), biomass burning (18.3%), plus soil dust (17.4%) comprise about two-thirds of the PM2.5 mass, followed by sulfate (6.5%). The sources of air pollution vary seasonally, particularly during the main wet season (June–September) and short rain season (February–April): From motor vehicles, (31.0 ± 2.6%) vs. (24.7 ± 1.2%); biomass burning, (21.5 ± 5%) vs. (14 ± 2%); and soil dust, (11 ± 6.4%) vs. (22.7 ± 8.4%), respectively, are amongst the three principal sources of ambient PM2.5 mass in the city. We suggest policy measures focusing on transportation, cleaner fuel or energy, waste management, and increasing awareness on the impact of air pollution on the public’s health.