Stored rainwater, the primary source of drinking water in the villages and towns of the Loess Plateau in northwest China, has been found to contain per- and polyfluoroalkyl substances (PFASs) and lacks necessary treatment measures. Coagulation is a common water treatment process, and enhancing its efficacy in removing PFASs can significantly improve treatment efficiency, reduce costs, and minimize the environmental and health risks associated with perfluorinated compounds. This study investigated the removal efficiency of perfluorobutanoic acid (PFBA), perfluorobutanesulfonic acid (PFBS), perfluorooctanoic acid (PFOA), and perfluorooctanesulfonic acid (PFOS) using inorganic salt coagulants alone and in combination with polydimethyldiallylammonium chloride (PDMDAAC). The results indicated that the removal efficiencies of the four PFASs by polyferric chloride (PFCl) and polyaluminum chloride (PACl) increased with alkalinity. PDMDAAC significantly enhanced the coagulation removal efficiency of the four PFASs. The removal efficiency of the four PFASs was highest when the raw water pH was near 7. Within the molecular weight range of 0–500,000 for PDMDAAC, the removal efficiency of the four PFASs increased with increasing molecular weight. Charge neutralization is the primary coagulation mechanism for the removal of anionic PFASs. Therefore, this study provides guidance for selecting coagulants to remove PFASs from stored rainwater.