There is a growing appreciation that engineered biointerfaces can regulate cell behaviors, or functions. Most systems aim to mimic the cell-friendly extracellular matrix environment and incorporate protein ligands; however, the understanding of how a ligand-free system can achieve this is limited. Cell scaffold materials comprised of interfused chitosan–cellulose hydrogels promote cell attachment in ligand-free systems, and these data were used to demonstrate the role of cellulose molecular weight (MW) and chitosan content and MW in controlling material properties and thus regulating cell attachment. Included are the data used for determining gel shear moduli; data used in cell attachment regression models and for determining average cell attachment; combined DAPI and FITC images of 24 hour cell morphology studies; data used for determining median cell aspect ratio, cell aspect ratio distribution, and median cell area; UV-vis adsorbance data; confocal microscopy data used for calculating chitosan penetration into cellulose gels; FTIR spectra data and fitted curves; scanning probe microscopy data used for determining gel surface roughness and capacitive coupling; and measurements of chitosan MW and gel surface zeta-potential