Phosphorus (P) management in the “water-energy-resource-nexus” in wastewater treatment plants (WWTPs) remains a longstanding challenge. P adsorption from the P-enriched digested sludge liquor (DSL) is a comparatively more practical and economically viable approach for P recovery in WWTPs. However, high concentrations of impurities in DSL might pose a negative and interferential effect on P adsorption, hindering the application of sorbents or precipitation methods. Given such a situation, highly efficient and cost-effective sorbent towards P reclamation from DSL is highly needed. Therefore, this study aims to develop a novel complex agent containing aluminum coagulant and superparamagnetic nano-sorbent (SNS) that can be used in magnetic seeding coagulation for P recovery. The complex agents with different PACl: SNS ratios showed varied turbidity removal rates and P recovery efficiencies and the optimal ratio was 15 mg PACl: 15 g SNS. PAC and SNS showed significant interaction because PAC could enhance P adsorption by shielding the interferential effect of colloidal impurities. In addition, the complex is highly regenerative, with turbidity and P removal rate stably maintained at 70–80% after 10 adsorption/regeneration cycles. The cost–benefit analysis of the dosing complex agent showed a dosing cost of 0.154 EUR/m3, admittedly much higher than the conventional magnetic seeding coagulation, which could probably be covered by the profit if the expensive and rare P product is reclaimed. This work indicated that the complex agent was superior due to its high adsorption capacity, easy separation, and repeated dosing, and therefore had the potential for P recovery from DSL.