A new attapulgite/UiO-66-NH2 composites adsorbent was prepared via solvothermal method and utilized to remove the Cr(VI) in the aqueous solution. The attapulgite/UiO-66-NH2 composites were detected by XRD, FTIR and SEM. The adsorption properties of the new adsorbent were investigated by batch experiments. The actual maximum removal efficiency was 96.31% at the optimal pH of 2 in 10 min, and the removal rate was directly proportional to the square of Cr ions concentration. Moreover, compared with UiO-66-NH2 and attapulgite, the attapulgite/UiO-66-NH2 composites adsorbent demonstrated an outstanding adsorption for Cr(VI). These results manifested that the attapulgite/UiO-66-NH2 composites were a latent adsorbent for the efficient removal of Cr(VI) in wastewater.