In this work, microcrystalline cellulose (MCC) was isolated from jute sticks and sodium carboxymethyl cellulose (Na-CMC) was synthesized from the isolated MCC. Na-CMC is an anionic derivative of microcrystalline cellulose. The microcrystalline cellulose-based hydrogel (MCCH) and Na-CMC-based hydrogel (Na-CMCH) were prepared by using epichlorohydrin (ECH) as a crosslinker by a chemical crosslinking method. The isolated MCC, synthesized Na-CMC, and corresponding hydrogels were characterized by Fourier transform infrared (FTIR), X-ray diffraction (XRD), scanning electronic microscopy (SEM), and energy dispersive spectroscopy (EDS) for functional groups, crystallinity, surface morphology, and composite elemental composition, respectively. Pseudo-first-order, pseudo-second-order, and Elovich models were used to investigate the adsorption kinetics. The pseudo-second-order one is favorable for both hydrogels. Freundlich, Langmuir, and Temkin adsorption isotherm models were investigated. MCCH follows the Freundlich model (R2 = 0.9967), and Na-CMCH follows the Langmuir isotherm model (R2 = 0.9974). The methylene blue (MB) dye adsorption capacities of ionic (Na-CMCH) and nonionic (MCCH) hydrogels in different contact times (up to 600 min), initial concentrations (10-50 ppm), and temperatures (298-318 K) were investigated and compared. The maximum adsorption capacity of MCCH and Na-CMCH was 23.73 and 196.46 mg/g, respectively, and the removal efficiency of MB was determined to be 26.93% for MCCH and 58.73% for Na-CMCH. The Na-CMCH efficiently removed the MB from aqueous solutions as well as spiked industrial wastewater. The Na-CMCH also remarkably efficiently reduced priority metal ions from an industrial effluent. An effort has been made to utilize inexpensive, readily available, and environmentally friendly waste materials (jute sticks) to synthesize valuable adsorbent materials.