Dyes are a type of pollutant that have been discharged into water streams by various industries and had harmful effects on the environment and human health. Therefore, present work was directed to recycle acrylic fibers waste to be used as an adsorbent to exclude dyes such as methylene blue (MB) and Congo red (CR) from dyes-polluted wastewater. Acrylic fibers waste was converted into membrane followed by chemical grafting with p-phenylenediamine monomer to form functional modified membranes. Afterwards, some characterization analyses; Fourier transform-infrared, scanning electron microscope, swelling behavior, and porosity properties were performed for the acrylic fiber grafted membrane (AFGM). For obtaining the best conditions that permit the highest adsorption capacity of the AFGM, some preliminary experiments followed by general full factorial design experiments were displayed. Langmuir, Freundlich isotherms and kinetic studies evaluations were applied. Results revealed that, the adsorption capacities of the AFGM were 61% for Methylene blue and 86% for Congo red that stated the high affinity of the AFGM to the anionic dyes. The reusability of the AFGM membranes in different cycles for 3Rs processes “Removal, Recovery, and Re-use” indicated the efficiency of the AFGM to be used in wastewater treatment.