The valorization of paper mill sludge (PMS) is the main goal of this study. The emissions of PMS continue to increase at global scale, especially from packaging paper and board sectors. The raw sludge was used to prepare an adsorbent to remove toxic pollutants from wastewater, the methylene blue (MB), an organic dye. Firstly, the physico-chemical characterization of PMS was done determining the crystalline phases of PMS fibers, the content of main elements, and the pH zero point charge, which was determined at around pH 7. The adsorption of MB on PMS powder was studied at 18 °C with an agitation of 200 rpm, being the best operating conditions 30 min of contact time, 250 mg L−1 of initial MB concentration and 0.05 g in 25 mL of adsorbent dose. Experimental data of MB adsorption was fitted to Langmuir and Freundlich isotherm equations. The Langmuir model was more accurate for the equilibrium data of MB adsorption at pH 5.1. The PFOM and PSOM were adjusted to experimental adsorption kinetics data, being PSOM, which describes better the MB adsorption by PMS powder. This was confirmed by calculating the maximum adsorption capacity with PSOM, which was 42.7 mg g−1, being nearly similar of the experimental value of 43.5 mg g−1. The analysis of adsorption thermodynamics showed that the MB was adsorbed exothermically with a ΔH0 = − 20.78 kJ mol−1, and spontaneously with ΔG0 from − 0.99 to − 6.38 kJ mol−1 in the range of temperature from 291 to 363 K, respectively. These results confirm that the sludge from paper industry can be used as biosorbent with remarkable adsorption capacity and low cost for the treatment of wastewater. PMS can be applied in the future for the depollution of the effluents from the textile industry, which are highly charged with dyes.