A lignocellulose@ activated clay (Ln@AC) nanocomposite with a hierarchical nanostructure was successfully synthesized by the chemical intercalation reaction and applied in the removal of Zn(II) from an aqueous solution. Ln@AC was characterized by N2 adsorption/desorption isotherms and X-Ray Diffraction (XRD), scanning Electron Microscope (SEM), transmission Electron Microscopy (TEM) and Fourier Transform Infrared Spectroscopy (FTIR) analysis, and the results indicate that an intercalated–exfoliated hierarchical nanostructure was formed. The effects of different adsorption parameters on the Zn(II) removal rate (weight ratio of Ln to AC, Ln@AC dosage, initial Zn(II) concentration, pH value, adsorption temperature, and time) were investigated in detail. The equilibrium adsorption capacity reached 315.9 mg/g under optimal conditions (i.e., the weight ratio of Ln to AC of 3:1, Ln@AC dosage of 1 g/L, initial Zn(II) concentration of 600 mg/L, pH value of 6.8, adsorption temperature of 65 °C, and adsorption time of 50 min). The adsorption process was described by the pseudo-second-order kinetic model, Langmuir isotherm model, and the Elovich model. Moreover, Zn(II) could be easily eluted by HCl, and the effects of HCl concentration, desorption temperature, and ultrasonic desorption time on desorbed amount were tested. Desorption studies revealed that with an HCl concentration of 0.25 mol/L, desorption temperature of 70 °C, and ultrasonic desorption time of 20 min, the maximum desorption capacity and efficiency were achieved at 202.5 mg/g and 64.10%, respectively. Regeneration experimental results indicated that the Ln@AC exhibited a certain recyclable regeneration performance. Due to such outstanding features, the novel Ln@AC nanocomposite proved to have great adsorption potential for Zn(II) removal from wastewater, and exhibited an extremely significant amount of adsorbed Zn(II) when compared to conventional adsorbents.