Cadmium (Cd) pollution in wastewater has become an increasingly widespread concern worldwide. Studies on Cd (II) removal using phosphate-adsorbed sorbents are limited. This study aimed to elucidate the behaviors and mechanisms of Cd (II) sorption on phosphate-loaded Ca-Mn-impregnated biochar (P_s-CMBC). The Cd (II) sorption on P_s-CMBC reached equilibrium within 2 h and exhibited a higher sorption efficiency than biochar and CMBC. Additionally, the Langmuir isotherm could better describe the Cd (II) adsorption on the sorbents. P₇₅-CMBC had a maximum Cd (II) sorption capability of 70.13 mg·g⁻¹ when fitted by the Langmuir isotherm model, which was approximately 3.18 and 2.86 times greater than those of biochar and CMBC, respectively. Higher pH (5–7) had minimal effect on Cd (II) sorption capacity. The results of characterization analyses, such as SEM-EDS, FTIR, and XPS, suggested that there was a considerable difference in the sorption mechanisms of Cd (II) among the sorbents. The primary sorption mechanisms for biochar, CMBC, and P_s-CMBC included electrostatic attraction and surface complexation; additionally, for P_s-CMBC, Cd (II)-π interactions and coordination of Cd (II) with P=O were critical mechanisms for Cd (II) removal. The results of this study demonstrate that phosphate-loaded CMBC can be used as an effective treatment for heavy metal pollution in aqueous media.