In this study, cellulose nanocrystals (CNCs) were produced from pea peels by acid hydrolysis to be used with pectin and acrylic acid (AAc) to form Pectin-PAAc/CNC nanocomposite by γ-irradiation. The structure, morphology, and properties of the nanocomposite were investigated using Fourier transform infrared spectroscopy (FTIR) and atomic force microscopy (AFM) techniques. The nanocomposite hydrogel was used for the removal of methylene blue dye (MB) from wastewater. The results revealed that the presence of CNCs in the polymeric matrix enhances the swelling and adsorption properties of Pectin-PAAc/CNC. The optimum adsorbate concentration is 70 mg/L. The kinetic experimental data were fit by pseudo-first-order (PFO), pseudo-second-order (PSO), and Avrami (Avr) kinetic models. It was found that the kinetic models fit the adsorption of MB well where the correlation coefficients of all kinetic models are higher than 0.97. The Avr kinetic model has the lowest ∆qe (normalized standard deviation) value, making it the most suitable one for describing the adsorption kinetics. The adsorption isotherm of MB by Pectin-PAAc follows the Brouers–Sotolongo model while that by Pectin-PAAc/CNC follows the Langmuir isotherm model. The negative values of ∆G confirmed the spontaneous nature of adsorption, and the positive value of ∆H indicated the endothermic nature of the adsorption.