With the growing need for high-purity rare-earth elements (REEs), the separation of these REEs has received much attention recently. The objective of this research is to produce chitosan from shrimp waste, then modify it with different functionality, and investigate the adsorption properties of chitosan adsorbents towards La(III) ions. First, from shrimp waste, chitosan (ch) with a significant degree of deacetylation, purity, and solubility was produced. The purified chitosan was cross-linked with epichlorohydrin (ep), and then, it was modified with 3,6,9,12-tetraazatetradecane-1,14-diamine (HA) to produce polyaminated chitosan (HA@ep@Ch). The polycarboxylated/imine chitosan (CM@HA@ep@Ch) was obtained by treating polyaminated chitosan with chloroacetic acid in isopropyl alcohol. The chitosan adsorbents were characterized and applied for lanthanum recovery from synthetic and monazite leach liquor samples. The factors controlling the recovery process were studied and discussed. The performance of the adsorbents was achieved through equilibrium, dynamic, and isothermal studies. HA@ep@Ch and CM@HA@ep@Ch showed good performance for lanthanum recovery with a maximum capacity of 114.52 and 141.76 mg/g at 330 K, respectively. The isotherm parameters refer to the monolayer of lanthanum adsorbed into the adsorbents through chelation and ion exchange mechanisms. A 0.5-M HCl solution was found effective to elute 95.8% of the adsorbed lanthanum on HA@ep@Ch, and 93.4% of the adsorbed lanthanum on CM@HA@ep@Ch. The adsorbents showed greater selectivity in extracting La, Ce, Pr, Nd, and Sm (62–75%) from REE leach liquid compared to extracting other REEs (20–41%).