Lignocellulose (LCE) was ultrasonically treated and intercalated into magnesium aluminum silicate (MOT) clay to prepare a nano-lignocellulose magnesium aluminum silicate polymer gel (nano-LCE-MOT) for the removal of Zn (II) from aqueous solution. The product was characterised using nitrogen adsorption/desorption isotherm measurements, Fourier-transform infrared spectroscopy, scanning electron microscopy and energy-dispersive X-ray spectroscopy. The conditions for the adsorption of Zn (II) on nano-LCE-MOT were screened, and adsorption kinetics and isotherm model analysis were carried out to explore the adsorption mechanism and achieve the optimal adsorption of Zn (II). Optimal adsorption was achieved at an initial Zn (II) concentration of 800 mg/L at 60 °C in 160 min at a pH of 4.52. The adsorption kinetics were explored using a pseudo-second-order model, with the isotherm adsorption equilibrium found to conform to the Langmuir model. The maximum adsorption capacity of the nano-LCE-MOT polymer gel toward Zn (II) is 513.48 mg/g. The materials with adsorbed Zn (II) were desorbed using different media, with HCl found to be the most ideal medium to desorb Zn (II). The optimal desorption of Zn (II) was achieved in 0.08 mol/L HCl solution at 65 °C in 60 min. Under these conditions, Zn (II) was almost completely desorbed from the adsorbents, with the adsorption effect after cycling being slightly different from that of the initial adsorption.