Air pollution caused by particulate matter (PM) has become a serious issue, and significant research has focused on managing large stationary emission sources, i.e., the primary sources of PM. Currently, the U.S. Environmental Protection Agency (EPA) Method 201A and ISO 23210 are predominantly employed to measure the PM emissions at large stationary sources. Method 201A is designated as a standard test method in Korea, but it is difficult to measure PM10 and PM2.5 simultaneously owing to the size of the full-set cyclone. In large stationary emission sources, the use of a serial connection of PM10 and PM2.5 cyclones is unsuitable for measurements at conventional sampling ports featuring diameters of approximately 100 mm. Therefore, in this study, PM10 and PM2.5 cyclones were developed to replace the cyclones currently used in Method 201A. The developed cyclones featured a cutoff diameter, which was confirmed by numerical and experimental analyses that were close to Method 201A. Moreover, there was an increase in the stiffness of collection efficiency. The hook adaptor, which is a key accessory used in Method 201A, was found to be applicable to the newly developed cyclones. This alternative method will help reduce the measurement time by simultaneously measuring TSP, PM10, and PM2.5 and eliminates the costs of installing or refurbishing additional sampling ports at existing large stationary sources.