In this work, crystalline cellulose (CC) was extracted from sugarcane bagasse through a facile modification method and further applied to absorb crystal violet dye (CV) in aqueous media. The proposed modification approach uses a mixture of NaOH and H2O2 only in a two‐step extraction process. This method is more straightforward than previous extraction methods, which used complex mixtures of solvents and additives. The yield obtained was 76.90%, approximately higher than several works declared before. The as‐prepared product was then determined with Fourier transform infrared spectroscopy (FT‐IR) and X‐ray diffraction (XRD) to analyze the presence of the functional groups and crystallinity, respectively. Furthermore, surface morphology, specific surface area of 0.634 m2 g−1, pore diameters of 3.010 nm, and pore size distribution of the obtained CC were determined with scanning electron microscope (SEM) and Brunauer–Emmett–Teller (BET) methods from the nitrogen adsorption–desorption isotherm, respectively. Additionally, serial experiments were conducted to investigate the influence of pH on the CV removal process. The results showed that the extracted material had a wide operating pH range of 6.0–9.0 and exhibited the highest CV treatment ability at pH 7.0. Besides, the effect of the parameters on the CV removal abilities, such as contact time (1–90 min), adsorbent dose (0.01–0.5 g), and initial CV concentration (10–100 mg L−1), was also investigated. To evaluate the CV removal ability of extract CC in the aqueous media and propose a suitable adsorption mechanism, we used several adsorption isotherms and adsorption kinetic models, such as Langmuir, Freundlich, Temkin, and Elovich. The obtained results showed that the adsorbent followed the pseudo‐second‐order kinetic model. Moreover, according to the Langmuir adsorption isotherm model, the maximum CV adsorption capacity (qm) of the CC was 8.857 mg g−1. Thermodynamic parameters such as −20 < ΔG0 < 0 (kJ mol−1), ΔH0 was 29.500 kJ mol−1, and the positive ΔS0 proved that the CV adsorption process of the CC was physical adsorption, spontaneous and endothermic. Overall, this study offers a simple approach based on the acid hydrolysis method for the high‐value utilization of sugarcane bagasse to isolate CC. This obtained product could become an active adsorbent for removing CV from the aqueous solutions.