•New adsorbents were prepared by combining chitosan and poly(1-vinylimidazole) using a facile technique.•High adsorption capacity was observed with the new adsorbent.•Synergistic effect was realized from chitosan and poly(1-vinylimidazole).•Interaction mechanism was also evaluated. Chitosan and poly(1-vinylimidazole) are both potential adsorbents to remove Cr(VI). Here, we designed the preparation of new adsorbents by combining chitosan and poly(1-vinylimidazole) to get the synergistic effect for the removal of hexavalent chromium. Trimethoxysilyl group terminated poly(1-vinylimidazole)-modified-chitosan composite was successfully synthesized by one-step free radical polymerization based on the grafting backbone of chitosan and vinylimidazole. The resulting adsorbents were used for the removal of Cr(VI) ions from the aqueous solution. The modified chitosan composite was characterized by ATR, FTIR, BET isotherm studies, elemental analysis, TGA, DSC, FE-SEM, and EDX. ATR. FTIR results confirmed the presence of the imidazole group in modified chitosan. The adsorption results were described by the Langmuir isotherm model with a maximum adsorption capacity of 196.1 mg/g for modified chitosan, however, the chitosan yielded 151.5 mg/g. It has been observed that the adsorption of chromium fitted better with the pseudo-second-order kinetics. The modified chitosan composite exhibited greater adsorption capacity than chitosan for hexavalent chromium and has potential application for Cr(VI) removal from aqueous solution containing other common ions with regeneration ability. This novel approach of modifying chitosan with telomerized poly(1-vinyl imidazole) offers potential application in wastewater treatment of different industries releasing Cr (VI).