Great efforts have long been made to control sediment pollution from persistent organic pollutants and phosphorus for aquatic ecosystem restoration. This study proposed a novel recycling of drinking water treatment residue (DWTR) to synchronously control sediment polycyclic aromatic hydrocarbons (PAHs) and phosphorus pollution based on a 350-day incubation test. The results suggested that DWTR addition reduced approximately 88%− 96% of potential bioavailable PAHs and 76% of mobile phosphorus in sediment. The dominant mechanisms for both reductions by DWTR were immobilization, mainly through increasing sediment amorphous aluminum and iron. The tendency of enhanced PAHs degradation by DWTR was also observed, especially for high molecular weight PAHs (e.g., chrysene, indeno(1, 2, 3-cd)pyrene, and benzo(g, hi)perylene), which decreased by approximately 21.1%− 22.0% of the total. Additionally, accompanying a clear increase in the connections of microbial cooccurrence networks, the variations in bioavailable PAHs, amorphous aluminum and iron, and other properties (e.g., pH, nitrogen, and organic matter) significantly (p < 0.01) enhanced Flavobacterium enrichment, although the enrichment of many other microbes potentially related to PAHs degradation (e.g., C1-B045) decreased after DWTR addition. Therefore, DWTR could promote the construction of a “PAHs immobilization with microbial augmentation” system while immobilizing phosphorus in sediment, indicating the high feasibility of controlling multiple sediment pollution.