The overall objective of this research was to investigate various methods and parameters to increase the efficiency of chemically enhanced primary treatment (CEPT). The performance of CEPT was evaluated based on its efficiency of removal of nonsettleable solids (NSS). Some of the source characteristics that influenced NSS concentration included influent total suspended solids, influent turbidity, and influent total chemical oxygen demand. A higher concentration of the influent constituents led to a higher NSS concentration, suggesting that NSS represented a somewhat fixed fraction or percent of these influent constituents. The specific particle surface area (SPSA) was found to correlate with percent NSS in the effluent. A higher SPSA is a result of smaller-sized nonsettleable colloidal particles, thus leading to an increase in percent NSS. In summary, there are several parameters that affect NSS, which could be used to control NSS to improve CEPT, as demonstrated by this study.