In this report, the adsorption of Cr(VI) onto MnO2/CS nanocomposite material from aqueous solution is investigated. All the factors, which affect the adsorption, such as pH, adsorption time, Cr(VI) initial concentration and adsorbent dosage, are also examined. The results obtained show that the Cr(VI) uptake is strongly affected by pH and ion strength. Analysis within the nonlinear isotherm models indicates that the Sips isotherm combining with the Langmuir and Freundlich models offer the best fit to the experimental data due to the obtained highest R2 and smallest RMSE and χ2 values. The calculated Langmuir monolayer adsorption capacity is 61.56 mg g−1 at pH of 2.0 and adsorption time of 120 min. Moreover, the mechanism studies by combining theoretical models with analytical spectroscopies reveal that the electrostatic attraction plays the important role to the uptake of Cr(VI) onto MnO2/CS nanocomposite. Therefore, the present nanocomposite material can be applied to remove total Cr from wastewater produced by the galvanized manufacturing factory with a relatively high efficiency. Display omitted •MnO2/CS nanocomposite was used as an adsorbent to remove Cr(VI) from aqueous solution.•The Langmuir monolayer adsorption capacity is 61.56 mg g−1.•The primary mechanism of the uptake of Cr(VI) onto MnO2/CS was proposed.•MnO2/CS was applied to remove total Cr in effluent with the high removal of 94.21%.