Increased phosphate concentration in water bodies has led to eutrophication, and its removal is an inevitable requirement of sustainable wastewater purification systems. In this study, MgAl layered doubled hydroxide (LDH) composites doped on the surface of activated carbon (AC/MgAl LDH) with various (Mg + Al) total metal loading (5 wt%, 10 wt%, and 15 wt%) were prepared by the co-precipitation method. The influence of (Mg + Al) total metal loading onto AC was examined to remove phosphate ions from aqueous solutions. The effect of adsorption parameters, including adsorbent dosage, initial solution pH, initial phosphate concentration, contact time, and experiment temperature, were investigated via batch adsorption experiments. The adsorption results demonstrated that the phosphate adsorption capacity significantly improved with increasing the (Mg + Al) metal loading on the surface of AC. The maximum Langmuir phosphate adsorption capacity was 337.2 mg phosphate per gram of AC/MgAl-3 LDH composite (15 wt% Mg + Al) composite at pH ~6.3, 22 °C, and 1 g/L of adsorbent. The kinetic data were best fitted with the pseudo-second order model. The initial solution pH notably influenced the phosphate removal by AC/MgAl-3 LDH composite with a maximum removal at pH 2.3. According to the spent adsorbent characterization results, the dominant mechanisms of phosphate removal by AC/MgAl-3 LDH were electrostatic interactions, ion exchange, and inner-sphere complexation. The phosphate adsorption capacity was gradually increased with increasing the experiment temperature, suggesting an endothermic adsorption process. Overall, the AC/MgAl LDH composites pave the way for an effective strategy for phosphate removal from aqueous solutions.