Cellulosic woven waste was used as a biomass material to prepare a Cu-doped BTC (Cu-BTC) adsorbent, which was then used to remove methylene blue (Basic Blue 9) from wastewater. Cellulosic woven waste was used as a biomass material to prepare a Cu-doped BTC (Cu-BTC) adsorbent, which was then used to remove methylene blue (Basic Blue 9) from wastewater. The Cu-BTC had higher adsorption capacity for methylene blue (BB9) than pure woven waste because it had high specific surface area and electrostatic interaction with cationic methylene blue molecules. The Cu-BTC removed methylene blue from wastewater rapidly and effectively and had an excellent adsorption capacity (197.90 mg/g). In batch process, the adsorption efficiency of the adsorbent for removal of BB9 was evaluated within 20 °C-60 °C, with initial BB9 concentrations of 50−200 mg/L and initial pH of 2−11. The Cu-BTC activation tailored the topological and textural properties of the obtained adsorbent, leading to a relatively large surface area of 1418.3 m 2 /g and pores with a volume of 0.491 cm 3 /g and an average size of 2.11 nm. The adsorption process fitted well with the Langmuir isotherm and the pseudo-second-order kinetic model. The possible mechanism for methylene blue removal mainly involved electrostatic attraction and micro pores. This study can serve as a guide for value-added utilization of cellulosic woven waste and as a practical method for the removal of methylene blue from wastewater. Adsorption of methylene blue onto the Cu-BTC is an effective and eco-friendly method for its removal from wastewater.