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Source and ambient samples were collected in a city in China that uses considerable biofuel, to assess influence of biofuel combustion and other sources on particulate matter (PM). Profiles and size distribution of biofuel combustion were investigated. Higher levels in source profiles, a significant increase in heavy-biomass ambient and stronger correlations of K+, Cl−, OC and EC suggest that they can be tracers of biofuel combustion. And char-EC/soot-EC (8.5 for PM2.5 and 15.8 for PM10 of source samples) can also be used to distinguish it. In source samples, water-soluble organic carbon (WSOC) were approximately 28.0%–68.8% (PM2.5) and 27.2%–43.8% (PM10) of OC. For size distribution, biofuel combustion mainly produces smaller particles. OC1, OC2, EC1 and EC2 abundances showed two peaks with one below 1 μm and one above 2 μm. An advanced three-way factory analysis model was applied to quantify source contributions to ambient PM2.5 and PM10. Higher contributions of coal combustion, vehicular emission, nitrate and biofuel combustion occurred during the heavy-biomass period, and higher contributions of sulfate and crustal dust were observed during the light-biomass period. Mass and percentage contributions of biofuel combustion were significantly higher in heavy-biomass period. The biofuel combustion attributed above 45% of K+ and Cl−, above 30% of EC and about 20% of OC. In addition, through analysis of source profiles and contributions, they were consistently evident that biofuel combustion and crustal dust contributed more to cation than to anion, while sulfate & SOC and nitrate showed stronger influence on anion than on cation.