Nanocellulose shows potential as an effective natural adsorbent for removing harmful contaminants from wastewater. This paper describes the development of innovative nanocellulose thin films made of cellulose nanocrystals (CNCs), polyacrylic acid (PAA), and active carbon (AC) as adsorbent materials for absorbing azo dyes from wastewater. The CNCs were recovered from sugarcane bagasse using alkali treatment and acid hydrolysis. The composition and processing parameters of the thin films were optimized, and their adsorption capacity was determined using thermodynamic isotherms and adsorption kinetics. Adsorption characteristics such as the methylene blue (MB) dye concentration, contact time, temperature, and pH were investigated to determine how they affected adsorption. The results show that the adsorption process follows pseudo-second-order kinetics. At an adsorbent mass of 50 mg, dye concentration of 50 ppm in 50 mL, and contact period of 120 min at 25 °C, the thin film comprising 64 wt% CNC, 16 wt% PAA, and 20 wt% AC showed high dye removal efficiency (86.3%) and adsorption capacity (43.15 mg/g). The MB removal efficiency increased to 95.56% and the adsorption capacity to 47.78 mg/g when the medium’s pH was gradually increased from neutral to alkaline. The nontoxicity, low production cost, water stability, easy recovery, and high adsorption capacity of these membranes make them suitable for water treatment systems.