Cu(PABA) is a Cu-based MOF material assembled from Cu2+ and the organic ligand p-aminobenzoic acid (PABA). Cu (PABA) was synthesized by a solvothermal method, characterized and applied to the adsorption of direct red 31 dye (DR-31). The effects of pH, DR-31 concentration and temperature on the adsorption performance of Cu(PABA) were investigated. The adsorption kinetics were analyzed by pseudo-first-order, pseudo-second-order and intra-particle diffusion models, and the adsorption equilibrium data was fitted by Langmuir and Freundlich isotherm models. The pseudo-first-order kinetics and Langmuir model satisfactorily described the adsorption kinetics and adsorption equilibrium, respectively. The maximum adsorption capacity of Cu(PABA) for DR-31 dye at room temperature was 1,244.8 mg/g, as calculated using the Langmuir adsorption isotherm model. By response surface methodology (RSM), the optimal adsorption was found at pH value of 10.9, DR-31 dye concentration of 216.6 mg/L, and temperature of 27 °C, and the removal rate was as high as 99.4%. Therefore, Cu(PABA) can be used as an efficient adsorbent for removing DR-31 dye from aqueous solution.