Biosorption using agricultural wastes has been proven as a low cost and efficient way for wastewater treatment. Herein, grape peel treated by microwave- and conventional-hydrothermal processes was used as low cost biosorbent to remove methylene blue (MB) from aqueous solutions. The adsorption parameters including the initial pH value, dosage of biosorbents, contact time, and initial MB concentration were investigated to find the optimum adsorption conditions. The biosorbent obtained by microwave-hydrothermal treatment only for 3 min at 180 °C (microwave-hydrothermal treated grape peel, MGP) showed faster kinetics and higher adsorption capability than that produced by a conventional-hydrothermal process (hydrothermal treated grape peel, HGP) with a duration time of 16 h. The maximum adsorption capability of MGP under the optimum conditions (pH = 11, a dosage of 2.50 g/L) as determined with the Langmuir model reached 215.7 mg/g, which was among the best values achieved so far on biosorbents. These results demonstrated that the grape peel treated by a quick microwave-hydrothermal process can be a very promising low cost and efficient biosorbent for organic dye removal from aqueous solutions.