The efficacy of plastic particle removal by municipal water treatment plants is currently uncertain, and the mechanisms involved in microplastic (MP) coagulation and flocculation have only been superficially investigated. The removal of pristine versus weathered plastic debris and the impact of plastic particle size on removal remain largely unexplored. In this study, coagulation, flocculation, and settling performances were investigated using pristine and weathered MPs (polyethylene (PE) and polystyrene (PS) microspheres, and polyester (PEST) fibers). Weathering processes that changed the surface chemistry and roughness of MPs impacted MP affinity for coagulants and flocculants. A quartz crystal microbalance with dissipation monitoring was used to identify the mechanisms involved during MP coagulation and flocculation. Measured deposition rates confirmed the relatively low affinity between plastic surfaces and aluminum-based coagulants compared to cationic polyacrylamide (PAM). In every case examined, coagulant efficiency increased when the plastic surface was weathered. Removals of 97 and 99% were measured for PEST and weathered PE, respectively. Larger pristine PE MPs were the most resistant to coagulation and flocculation, with 82% removal observed even under enhanced coagulation conditions. By understanding the interaction mechanisms, the removal of weathered MPs was optimized. Finally, this study explored the use of settled water turbidity as a possible indicator of MP removal.