Biopolymers are promising materials for water treatment applications due to their abundance, low cost, expandability, and chemical structure. In this work, gelatin hydrogels filled with cellulose in the form of pristine eucalyptus residues (PER) or treated eucalyptus residues (TER) were prepared for adsorption and chromium removal in contaminated water. PER is a lignocellulosic compound, with cellulose, hemicellulose, and lignin, while TER has cellulose as a major component. FT-Raman Spectroscopy and FTIR analysis confirmed the crosslink reaction with glutaraldehyde and indicated that fillers altered the gelatin molecular vibrations and formed new hydrogen bonds, impacting the hydrogels' crystalline structure. The hydrogen bond energy was altered by the cellulosic fillers' addition and resulted in higher thermal stability (~10 °C). Hydrogels presented a Fickian diffusion, where gelatin hydrogel showed the highest swelling ability (466%), and composites showed lower values with the filler content increase. The chromium adsorption capacity presented values between 12 and 13 mg/g, i.e., featuring an excellent removal capacity which is related with hydrogel crosslinked structure and fibers surface hydroxyl groups, highlighting gelatin hydrogel TER 5% with better removal capacity. The developed hydrogels were produced from biomacromolecules with low-cost and potential application in contaminated water.