Biosorption is a bioremediation approach for the removal of harmful dyes from industrial effluents using biological materials. This study investigated Methylene blue (M. blue) and Congo red (C. red) biosorption from model aqueous solutions by two marine macro-algae, Ulva fasciata and Sargassum dentifolium, incorporated within acrylic fiber waste to form composite membranes, Acrylic fiber-U. fasciata (AF-U) and Acrylic fiber-S. dentifolium (AF-S), respectively. The adsorption process was designed to more easily achieve the 3R process, i.e., removal, recovery, and reuse. The process of optimization was implemented through one factor at a time (OFAT) experiments, followed by a factorial design experiment to achieve the highest dye removal efficiency. Furthermore, isotherm and kinetics studies were undertaken to determine the reaction nature. FT-IR and SEM analyses were performed to investigate the properties of the membrane. The AF-U membrane showed a significant dye removal efficiency, of 88.9% for 100 ppm M. blue conc. and 79.6% for 50 ppm C. red conc. after 240 min sorption time. AF-S recorded a sorption capacity of 82.1% for 100 ppm M. blue conc. after 30 min sorption time and 85% for 100 ppm C. red conc. after 240 min contact time. The membranes were successfully applied in the 3Rs process, in which it was found that the membranes could be used for five cycles of the removal process with stable efficiency.