Recently, precursor gases such as ammonia have sparked a growing interest in the secondary formation of particulate matter (PM). Most studies focus on urban areas and scientific data. Studies on precursor gases and PM emitted from agricultural sources are insufficient; thus, this paper presents a field monitoring study conducted from agricultural sources. To estimate the effect of precursor gases for PM2.5 from naturally ventilated dairy barns, correlation analyses were conducted using real-time monitoring data on the mass concentrations of PM2.5, NH3, SO2, NO2, and H2S and meteorological data. In addition to mass concentration, the emission and loading rates were used to closely analyze pollution status. The mass concentrations of PM2.5 and gaseous compounds did not correlate well, whereas the mass emission rates for PM2.5 and gaseous compounds (SO2, NH3, and NO2) correlated well because the unit of the emission rate reflected the ventilation factor. The correlation coefficients between PM2.5 and precursor gas emission rates ranged from 0.72 to 0.89 (R), with the SO2 emission rate exhibiting the highest correlation coefficient (R = 0.89). This correlation implies that SO2 from dairy farms is a dominant species among the gaseous precursors influencing the secondary formation of PM2.5; alternatively, SO2 and PM2.5 are produced from the same sources. The ambient PM2.5 loading rate and barn PM2.5 emission rate—estimated by multivariate linear regression using the gaseous independent variables NH3, SO2, and NO2—revealed high-correlation coefficients (0.60 and 0.92, respectively) with the measured data. At present, most studies investigating the precursor gases of PM in agricultural fields have focused on NH3; however, this study suggests that SO2 is a key factor in PM2.5 pollution. To elucidate the secondary formation of PM from precursor gases in agricultural sources, particulate ammonium, sulfate, nitrate, and chloride, which were not measured in this study, as well as oxidants and intermediates, should be considered in future research.