Here, for the first time, neodymium was incorporated into the three-dimensional mesoporous siliceous material; TUD-1. In order to understand the chemical and morphological structure of the prepared material, several characterization techniques were performed. The characterization results showed the formation of highly distributed isolated Nd3+ ions incorporated in the silica matrix in tetrahedrally coordinated structure, moreover no aggregation of separate phase(s) was/were observed. The prepared material was investigated as an adsorbent for methyl green (MG) dye in aqueous solution as a model cationic dye. The results showed higher adsorption capacity for Nd-TUD-1 by almost 24 times higher than the neat parent TUD-1 material and more than 100 times higher than bulky Nd2O3 under neutral pH. The adsorption results were fitted perfectly with pseudo-second-order model. Moreover, the adsorption isotherms were perfectly fitted with Freundlich isotherm model which indicated the formation of a multilayer of the dye molecules onto the Nd-TUD-1 surface as a physisorption with endothermic nature.