We investigated the effects of the addition of two coagulants−polyaluminium chloride (PACl) and chitosan−into the membrane bioreactor (MBR) process on membrane fouling and the removal of pharmaceuticals and personal care products (PPCPs). Their addition at optimized dosages improved the permeability of the membrane by reducing the concentration of soluble microbial products in mixed liquor, the content of inorganic elements, and irreversible fouling of the membrane surface. During long-term operation, the addition of PACl increased removal efficiencies of tetracycline, mefenamic acid, atenolol, furosemide, ketoprofen, and diclofenac by 17–23%. The comparative evaluation using mass balance calculations between coagulation-MBR (with PACl addition) and control-MBR (without PACl addition) showed that enhanced biodegradability played a key role in improving removal efficiencies of some PPCPs in coagulation-MBR. Coagulation-MBR also had higher oxygen uptake rates and specific nitrification rates of microorganisms. Overall, our findings suggest that the combination of MBR with coagulation reduced membrane fouling, lengthening operation period of the membrane, and improved the removal of some PPCPs as a result of enhanced biodegradability.