A one-pot synthetic methodology for fabricating stimuli-responsive hemicellulose-based hydrogels was developed that consists of the in situ formation of magnetic iron oxide (Fe3O4) nanoparticles during the covalent cross-linking of O-acetyl-galactoglucomannan (AcGGM). The Fe3O4 nanoparticle content controlled the thermal stability, macrostructure, swelling behavior, and magnetization of the hybrid hydrogels. In addition, the magnetic field-responsive hemicellulose hydrogels (MERHHs) exhibited excellent adsorption and controlled release profiles with bovine serum albumin (BSA) as the model drug. Therefore, the MFRHHs have great potential to be utilized in the biomedical field for tissue engineering applications, controlled drug delivery, and magnetically assisted bioseparation. Magnetic field-responsive hemicellulose hydrogels, prepared using a straightforward one-step process, expand the applications of biomass-derived polysaccharides by combining the renewability of hemicellulose and the magnetism of Fe3O4 nanoparticles.