An adsorptive membrane filtration based on polyvinylidene fluoride (PVDF) with chitosan (CS) and carboxylated carbon nanotubes (CNTs-COOH) is prepared by method of phase conversion, and the PVDF-CS@CNTs-COOH membranes can effectively separate anionic and cationic dye wastewater. Compared to pure PVDF membranes, PVDF-CS@CNTs-COOH increases pure water flux from 36.39 (L·m-2·h-1) to 85.25 (L·m-2·h-1), an increase of nearly 230%. The membrane exhibits excellent rejection performance in the filtration of six types of dye wastewater. The modified membranes also performed well in terms of rejection of mixed anionic and cationic dyes and also have a high performance in recycling, with a flux of over 94% for both anionic and cationic dyes. In addition, the adsorption curve fitting results showed that the adsorption process was more consistent with the pseudo-second-order adsorption kinetic model and Langmuir mode.