UiO-66-NH2 was functionalized with an ionic polymer poly(2-acrylamido-2-methylpropane sulfonic acid) (PAMPS) through a post-synthetic modification (PSM) strategy. Due to the excellent dispersibility in water and the existence of abundant active binding sites, the obtained UiO-66-PAMPS shows significantly improved adsorption capability toward methylene blue (MB) in aqueous solution.