In order to produce efficient green adsorbent materials, neodymium alginate (SA/Nd) gel spheres were prepared by crosslinking sodium alginate reaction with rare earth ions using the droplet polymerization method. The prepared materials were characterized and analyzed by SEM-EDS, XRD, TGA, FT-IR, UV-Vis, BET-BJH and XPS, and the adsorption performance of SA/Nd on azo dyes in water was investigated. The results show that SA/Nd has a pleated structure with abundant oxygen-containing functional groups. The adsorption of 1200 mg/L of Direct Blue GL (DB 151) and Direct Orange 26 (DO 26) reached 1325 mg/L and 1175 mg/g, respectively, under the optimal conditions. After seven desorption and recycling of the adsorbent material, the removal rate of the two azo dyes remained above 80%. SA/Nd mainly realizes efficient adsorption of dyes through electrostatic, hydrogen bonding and complexation, and the above results can provide a reference for the treatment of printing and dyeing wastewater.