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Highly phosphorylated cellulose was produced under different processing parameters and used as an effective adsorbent for methylene blue (MB) dye removal from aqueous systems. The characteristics of the designed adsorbent were analyzed using different technics. The zeta potential measurement of the developed adsorbents was negative (-11.3 to -49.4 mV) in the pH range of 4 to 11. Batch removal tests were performed under different processing parameters of contact time, initial concentration, phosphorylation degree and pH. The developed adsorbent with a high substitution degree of 1.07 (13.22 % of P), revealed an outstanding retention capacity for MB dye (up to 3153.5 mg/g) during an extremely low equilibrium adsorption time (∼30 min), which is 130-fold higher than pure MCC (15.3 mg/g). Interestingly, this capacity raised up to 3236.6 mg/g when raising the pH of the solution (from 7 to 11). The experimental adsorption data in the examined conditions were well fitted by the Langmuir type isotherm and pseudo-second-order kinetic models, highlighting the significance of the reaction medium and phosphate content in determining the adsorbent's retention capacity. This investigation has demonstrated the potential of converting pure MCC into high value-added adsorbent for the efficient purification of organic dye from aqueous solutions., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier B.V. All rights reserved.)