In this study, a novel and cost-effective approach was employed to prepare an effective Pb(II) adsorbent. We synthesized highly porous CMCSB-SCB microbeads with multiple active binding sites by combining carboxymethylated chitosan Schiff base (CMCSB) and sugarcane bagasse (SCB). These microbeads were structurally and morphologically characterized using various physical, analytical, and microscopic techniques. The SEM image and N2-adsorption analysis of CMCSB-SCB revealed a highly porous structure with irregularly shaped voids and interconnected pores. The CMCSB-SCB microbeads demonstrated an impressive aqueous Pb(II) adsorption capacity, reaching a maximum of 318.21 mg/g, under identified optimal conditions: pH 4.5, 15 mg microbeads dosage, 30 min contact time, and Pb(II) initial concentration (350 mg/L). The successful adsorption of Pb(II) onto CMCSB-SCB beads was validated using FTIR, EDX, and XPS techniques. Furthermore, the experimental data fitting indicated a good agreement with the Langmuir model (R2 = 0.99633), whereas the adsorption kinetics aligned well with the pseudo-second-order model (R2 = 0.99978). The study also identified the Pb(II) adsorption mechanism by CMCSB-SCB microbeads as monolayer chemisorption.