Phoenix dactylifera leaf extract was immobilized within cross-linked polyvinyl alcohol (PVA) for the removal of methylene blue (MB) from aqueous solutions. The Ultraviolet-visible (UV-vis) and Fourier transform infrared spectroscopic techniques were utilized to shed light on the functional groups accountable for the adsorption process. The adsorption experiments were conducted as a function of different operating variables (contact time, adsorbent dosage, initial dye concentration, and pH value). The developed P. dactylifera/PVA matrix can be considered as a low-priced green adsorbent with high efficiency for the removal of MB from aqueous solution.