Removal of toxic dyes from wastewater has become a hot topic in both academic and industrial fields since there is growing concern about the threat of sewage to human health. Herein, we demonstrate that the three-dimensional porous polyacrylamide-phytic acid-polydopamine (termed as PAAM/PA/PDA) hydrogel can be served as reusable adsorbent with high efficiency for either anionic or cationic dyes. Using methyl blue (MB), methylene blue (YMB), methyl violet (MV) and neutral red (NR) as model dyes, we investigate the effect of pH, temperature, dye concentration, and PAAM/PA/PDA hydrogel mass on the adsorption. The experimental maximum adsorption capacities are more than 350.67 mg g−1 for four selected dyes. Adsorption kinetic and thermodynamic analysis suggests that the dyes are adsorbed on the PAAM/PA/PDA hydrogel through the strong π-π stacking and anion-cation interaction, and the adsorption process satisfies a pseudo-second-order model. Furthermore, the free-standing PAAM/PA/PDA hydrogel can be easily removed from water after adsorption process, and regenerated by adjusting solution pH values.