Arabica-coffee and Theobroma-cocoa agroindustrial wastes were treated with NaOH and characterized to efficiently remove Pb(II) from the aqueous media. The maximum Pb(II) adsorption capacities, qmax, of Arabica-coffee (WCAM) and Theobroma-cocoa (WCTM) biosorbents (qmax = 303.0 and 223.1 mg·g−1, respectively) were almost twice that of the corresponding untreated wastes and were higher than those of other similar agro-industrial biosorbents reported in the literature. Structural, chemical, and morphological characterization were performed by FT-IR, SEM/EDX, and point of zero charge (pHPZC) measurements. Both the WCAM and WCTM biosorbents showed typical uneven and rough cracked surfaces including the OH, C=O, COH, and C-O-C functional adsorbing groups. The optimal Pb(II) adsorption, reaching a high removal efficiency %R (>90%), occurred at a pH between 4 and 5 with a biosorbent dose of 2 g·L−1. The experimental data for Pb(II) adsorption on WACM and WCTM were well fitted with the Langmuir-isotherm and pseudo-second order kinetic models. These indicated that Pb(II) adsorption is a chemisorption process with the presence of a monolayer mechanism. In addition, the deduced thermodynamic parameters showed the endothermic (ΔH0 > 0), feasible, and spontaneous (ΔG0 < 0) nature of the adsorption processes studied.