Theobroma cacao agro-industrial waste (WTC) has been characterized and tested as an effective biosorbent to remove Cd(II) from aqueous media. At the optimum pH of 5.0, a maximum adsorption capacity of qe,max = 58.5 mg g−1 was determined. The structural and morphological characterization have been conducted by FTIR, SEM/EDX, and TGA measurements. The SEM/EDX results confirmed that the metals are adsorbed on the surface. C-O-C, OH, CH, NH, and C=O functional groups were identified by FTIR. TGA results were consistent with the presence of hemicellulose. Biosorption kinetics were rapid during the first 30 min and then reached equilibrium. The corresponding experimental data were well fitted to pseudo-first and -second order models, the latter being the best. The biosorption isotherm data were also well fitted to Temkin, Langmuir, and Freundlich models, showing that several sorption mechanisms may be involved in the Cd(II) biosorption process, which was characterized as exothermic (ΔH0 < 0), feasible, and spontaneous (ΔG0 < 0). In binary (Cd–Pb and Cd–Cu) and ternary (Cd–Pb–Cu) systems, Cu(II) and particularly Pb(II) co-cations exert strong antagonistic effects. Using HNO3, effective good regeneration of WTC was obtained to efficiently remove Cd(II) up to three times.