To analyze the physicochemical mechanisms affecting the variation in fine suspended particulate matter (PM2.5) concentrations in Taichung City, the largest city in central Taiwan (the second largest city in Taiwan), during a high-pollution event from November 3 to 6, 2021, we applied the sulfur tracking method (STM) and integrated source apportionment method (ISAM) of the WRF/CMAQ model to simulate the impacts of various emission sources. The sources of pollution in Taichung City are very similar, which shows that the impacts of point, line, and area sources should not be neglected in addition to the boundary conditions. SO42− is mainly generated from point emissions and the production of H2O2, Fe, Mn, and O3. NO3− is also mainly generated from point sources in Taichung City, with HNO3 being the main source at noon and ANO3 at other times of the day. NH4+ is mainly generated from area sources in Taichung City. OM is more complex, mainly originating from line sources in Taichung City and other sources, such as point/area emissions in Taichung City and other emissions from Changhua County. The most important mechanism is low-volatility/semivolatile oxidized combustion of OC at noon, followed by low-volatility/semivolatile POA, which is produced in the morning or evening. EC mainly originates from line sources in Taichung City and Changhua County. In other nearby counties, EC is dominated by local emission sources. In addition, when the concentration of PM2.5 is high, the Neutralization Ratio (NR) is high and PM2.5 is relatively neutral or slightly alkaline. On the contrary, when the concentration of PM2.5 is low, the NR is lower than 1 and the aerosol is acidic. Besides, this study used positive matrix factorization (PMF), which indicates that the PM2.5 at the UAPRS originated from eight kinds of pollution, namely, windblown dust, oil cracking, iron and steel industry, sea salt, transport, Cl− containing exhaust, biomass burning, fossil combustion containing abundant SO42− and the heavy oil refining and coal combustion industry. The direction of the source of pollution can be traced by a conditional bivariate probability function (CBPF). Overall, fossil fuel combustion, mainly involving sulfate, is the largest source of pollution, with the heavy oil refining and coal combustion industry contributing less, and the remaining factors contribute relatively evenly.