Poly(hydroxylmethyl methacrylate-co-glycidyl methacrylate) (p(HEMA-GMA)) macroporous cryogel with high density of epoxy groups was synthesized, and the epoxy groups of the cryogel were modified into phosphonate groups. The effects of dye concentrations, adsorption time, pH, salt concentration, and adsorption temperature on the adsorption of Direct Blue-53 (DB-53) and Reactive Blue-160 (RB-160) dyes were studied. The maximum adsorption capacity was found to be 245.3 and 155.8 mg/g (0.255 or 0.119 mmol/g) for the DB-53 and RB-160 dyes, respectively. The higher adsorption capacity achieved for the DB-53 compared with the RB-160 dye can result from the pendant primary amino groups of the DB-53 dye as well as the smaller size of the dye molecule. The Langmuir isotherm model and the pseudo-second-order kinetic model well described the experimental data. The p(HEMA-GMA)-PO(4)(2-)adsorbent has many operational advantages for the removal of pollutants. It could be a promising adsorbent to be used in industrial wastewater treatment.