The Ordos region in the southwestern part of Inner Mongolia experiences frequent PM concentrations in excess of the national PM2.5 air quality standards. In order to determine the key sources of PM2.5 contributing to these pollution episodes, the main sources of PM2.5 OC during elevated PM episodes in the Inner Mongolia were analyzed and compared with non-polluted days. This will provide insight to the main sources of particulate matter pollution during the high-pollution episodes and the effective seasonal strategies to control sources of particulate matter during months and with the highest PM concentrations that need to be controlled. The PMF source contributions to OC demonstrated that the industrial/coal combustion (4762.77 ± 1061.54 versus 2726.49 ± 469.75 ng/m3; p < 0.001) and mobile source factors (4651.14 ± 681.82 versus 2605.55 ± 276.50 ng/m3; p value < 0.001) showed greater contributions to the elevated concentrations during the episode. The spatial analysis of secondary organic carbon (SOC) factors, regional biomass burning, and biogenic sources did not show significant difference in the pollution episodes and the non-polluted months. In addition, the bivariate polar plots and CWT maps of the industrial/coal combustion and mobile illustrated a regional long-range transport patterns from the external sources to the study area, however, adjacent areas were mostly controlling the contributions of these factors during the PM elevated episodes. The SOC sources, regional biomass burning, and biogenic sources illustrated a regional long-range transport with similar locations found during the elevated pollution episodes compared to the normal situations.