Alum sludge is the sludge discharged from a sedimentation tank in a drinking water treatment plant when polymerized with poly-aluminum chloride (PAC). In this paper, granular alum sludge adsorbent (GASA) was manufactured using powdery alum sludge (PAS) as the raw material and methods such as gluing and pore-forming. The effects of different binders, pore-forming agents, roasting temperatures, and roasting times on the formation of GASA and its dephosphorization performance were investigated. Results showed that the optimum binder was AlCl3 at a mass ratio of 8%, and the best pore-forming agent was starch at a 4% dosage ratio. Meanwhile, the optimum roasting temperature and time were 500 °C and 2 hours, respectively. The specific surface area of GASA was 23.124 m2/g. Scanning electron microscopy suggested that GASA's surface became rough, particles became tight, and average pore size increased, with additional pore channels. P adsorption by GASA reached 0.90 mg/g. The effluent phosphorus concentration of actual tail water decreased to 0.49 mg/L and the removal rate reached 73.5% when the GASA dosage was 20 g/L. The findings of this study are important for the further development of a low-cost adsorbent material for P removal in the future.