Wheat arabinoxylan was treated with two α-arabinofuranosidases exhibiting different mode of action to create three different polymeric substrates. These three substrate preparations were characterized by xylopyranose backbone sugars that are (1) singly substituted by arabinose at C2 or C3, (2) doubly substituted by arabinose at C2 and C3, and (3) largely unsubstituted. All xylan preparations were grafted with glycidyl methacrylate using cerium ammonium nitrate and then evaluated in terms of graft yield and adsorption to cellulose surfaces. The highest graft yield was observed for the xylan preparation characterized by a largely unsubstituted xylopyranose backbone. Furthermore, QCM-D analyses revealed that grafted xylans exhibited a two-stage desorption pattern, which was not seen with the ungrafted xylans and was consistent with increased water sorption. Accordingly, this study demonstrates the potential of arabinofuranosidases to increase the yield and influence the viscoelastic properties of grafted xylans used as biobased cellulose coatings.