Thiol-lignocellulose sodium bentonite (TLSB) nanocomposites can effectively remove heavy metals from aqueous solutions. TLSB was formed by using-SH group-modified lignocellulose as a raw material, which was intercalated into the interlayers of hierarchical sodium bentonite. Characterization of TLSB was then performed with BET, FTIR, XRD, TGA, PZC, SEM, and TEM analyses. The results indicated that thiol-lignocellulose molecules may have different influences on the physicochemical properties of sodium bentonite, and an intercalated-exfoliated structure was successfully formed. The TLSB nanocomposite was subsequently investigated to validate its adsorption and desorption capacities for the zinc subgroup ions Zn(II), Cd(II) and Hg(II). The optimum adsorption parameters were determined based on the TLSB nanocomposite dosage, concentration of zinc subgroup ions, solution pH, adsorption temperature and adsorption time. The results revealed that the maximum adsorption capacity onto TLSB was 357.29 mg/g for Zn(II), 458.32 mg/g for Cd(II) and 208.12 mg/g for Hg(II). The adsorption kinetics were explained by the pseudo-second-order model, and the adsorption isotherm conformed to the Langmuir model, implying that the dominant chemical adsorption mechanism on TLSB is monolayer coverage. Thermodynamic studies suggested that the adsorption is spontaneous and endothermic. Desorption and regeneration experiments revealed that TLSB could be desorbed with HCl to recover Zn(II) and Cd(II) and with-HNO3 to recover Hg(II) after several consecutive adsorption/desorption cycles. The adsorption mechanism was investigated through FTIR, EDX and SEM, which demonstrated that the introduction of thiol groups improved the adsorption capacity. All of these results suggested that TLSB is an eco-friendly and sustainable adsorbent for the extraction of Zn(II), Cd(II) and Hg(II) ions in aqueous media.