Perfluorooctanesulfonic acid and its salts (PFOS) are emerging contaminants with long half-lives in water and human bodies. Accordingly, PFOS removal from water streams is required for controlling the PFOS pollution. To provide a simple PFOS separation technology, effects of three additives, powdered activated carbon (PAC), gelatin, and cetyltrimethylammonium bromide (CTAB), on the PFOS removal by coagulation with ferric chloride or aluminum sulfate were investigated in this study. As a result, coagulation with PAC or CTAB addition was effective in the PFOS removal, though the conventional coagulation and coagulation with gelatin addition were ineffective. A PFOS removal efficiency of over 90% was observed for the CTAB dose of over 1.6 μM (0.58 mg/L) and for the PAC dose of over 40 mg/L, and that of over 95% was achieved by the CTAB dose of over 2.4 μM (0.87 mg/L), when the initial PFOS concentration was 1.84 μM. The positive effect of CTAB would be caused by micelle formation, which was enhanced by both the association of hydrophobic tails and the electrostatic attraction of hydrophilic heads of PFOS and CTAB. Thus, a linear cationic surfactant of CTAB was concluded to be an effective additive for the PFOS removal by coagulation.