Maleic anhydride-diethylenetriamine grafted on starch (st-g-(MA-DETA)) was synthesized through graft copolymerization, and the different parameters (copolymerization temperature, reaction time, concentration of initiator and monomer concentration) affecting starch graft percentage were studied to achieve the maximum grafting percentage. The maximum grafting percentage was found to be 29.17%. The starch and grafted starch copolymer were characterized using XRD, FTIR, SEM, EDS, NMR, and TGA analytical techniques to describe copolymerization. The crystallinity of starch and grafted starch was studied by XRD, confirming that grafted starch has a semicrystalline nature and indicating that the grafting reaction took place typically in the amorphous region of starch. NMR and IR spectroscopic techniques confirmed the successful synthesis of the st-g-(MA-DETA) copolymer. A TGA study revealed that grafting affects the thermal stability of starch. An SEM analysis showed the microparticles are distributed unevenly. Modified starch with the highest grafting ratio was then applied to celestine dye removal from water using different parameters. The experimental results indicated that St-g-(MA-DETA) has excellent dye removal properties in comparison to native starch.