Polyamine chelating adsorbents have a good removal effect on dye wastewater. In this study, small molecule triethylenetetramine and macromolecular poly(ethylene imine) were selected as aminated reagent, and two kinds of aminated chitosan microspheres, TETA-CTSms and PEI-CTSms, were obtained by emulsion cross-linking method. The microspheres were fully characterized by FTIR, SEM, XRD, EDS and TGA. EDS results showed that the N content of the PEI-CTSms and TETA-CTSms microspheres increased significantly after the cross-linking reaction and can reach 5.7 wt% and 7.3 wt%, respectively. Adsorption experiments confirmed that TETA-CTSms and PEI-CTSms showed greater adsorption characteristics for anionic dye reactive yellow (RY) in aqueous solutions compared with CTSms, and the adsorption capacity per unit area was increased by 39.11% and 88.56%, respectively. The adsorption capacity of aminated microspheres for RY decreased with the increase of pH. The adsorption kinetics conformed to the pseudo-second-order model, and the adsorption process was in accordance with the Langmuir isotherm model. The negative value of Δ
G
confirmed that the adsorption process was spontaneous, and the dye adsorption was a multiple process dominated by chemical chelating and physical adsorption.