A synthetic flocculant of aluminum (Al) and iron (Fe) extracted from red mud (RM) has been widely used in sewage treatment, while the remaining RM residue has been ignored. This study aimed to synthesize polymeric aluminum ferric sulfate (PAFS) flocculant from RM by acid leaching and then use the acidified RM residue to produce an acid RM-based ceramsite (ARMC) by mixing bentonite, hydroxypropyl methylcellulose, and starch. Our results showed that sintering, reaction temperature, H2SO4 concentration, reaction time, and liquid-to-solid ratio had an obvious effect on the leaching of Al and Fe in RM, which was a necessary prerequisite for the efficient PAFS flocculants. At a PAFS dosage of 60 mg/L, turbidity and phosphate removal rates were 95.21 ± 0.64% and 89.17 ± 0.52%, respectively. When the pH value was 8.0, the turbidity and phosphate removal efficiency were 99.22 ± 0.66% and 95.98 ± 1.63%, respectively. Considering the adsorption capacity and mechanical properties, the best conditions for ARMC production included using 60% ARM and ceramsite calcination at 600 °C, with the BET surface area 56.16 m2/g and a pore volume of 0.167 cm3/g. Thermogravimetric analysis indicated that 400 °C was a reasonable preheating temperature to enhance the ARMC mechanical strength, as this temperature allows the removal of surface-adsorbed and constituent water. Under a scanning electron microscope, the ARMC appeared rough before adsorption, while relatively uniform pores occupied it after adsorption. Our conclusion will help to improve the zero-waste strategy of RM and speed up the industrial production of RM in flocculants as well as utilizing ARMC as a new type of adsorbent for phosphorus adsorption in sewage treatment.