This study reports on the removal of orthophosphate (P-i) by coagulation-flocculation with variable combinations of alum, biopolymers, and bioinass. The combinatorial effects of these coagulant aids were evaluated for single, binary, and ternary systems. The role of pH, component dosages, and p(i) concentration on the coagulation flocculation efficacy was evaluated. There was an optimal dosage of alum (30 mg/L) while alginate and chitosan were 15 mg/L. P-i removal was 86% for alum and 98% for ternary systems containing chitosan and alginate where [P-i] = 10-11 mg P-i/L. Pi removal for the alum-alginate-chitosan ternary system was more efficient than that for the binary systems; especially at pH 6-7, where reduced efficiency occurred at pH > 7.5. P-i removal was independent of concentration except at lower levels, [P-i] < 10 mg/L. The alum-refined oat hull binary system was 99% effective for P-i removal, especially when [P-i] = 25 mg/L, with greater removal over the use of oat hulls alone.