In this study, ryegrass straw agricultural residue (Lolium multiflorum L.) was employed as an adsorbent material to remove methylene blue (MB) dye from aqueous solutions. Four adsorbents were produced using phosphoric acid and pyrolysis as activating agents. The samples were analyzed with TGA, FTIR, SEM, and XRD techniques. A rapid adsorption of the MB was obtained with the ryegrass treated with 40% H3PO4, reaching equilibrium in 2 min. Moreover, a maximum adsorption capacity of 80.79 mg g−1 and a removal efficiency of 99% were achieved. The results demonstrate a good performance of adsorbents from ryegrass for removing dye contaminants, such as methylene blue, from the aqueous solutions.