The purpose of this research is to develop strong and tough wood-based hydrogels, which are reinforced by an aligned cellulosic wood skeleton. The hypothesis is that improved interfacial interaction between the wood cell wall and a polymer is of great importance for improving the mechanical performance. To this end, a facile and green approach, called ultraviolet (UV) grafting, was performed on the polyacrylamide (PAM)-infiltrated wood skeleton without using initiators. An important finding was that PAM-grafted cellulose nanofiber (CNF) architectures formed in the obtained hydrogels under UV irradiation, where CNFs themselves serve as both initiators and cross-linkers. Moreover, an alkali swelling treatment was utilized to improve the accessibility of the wood cell wall before UV irradiation and thus facilitate grafting efficiency. The resulting alkali-treated Wood-g-PAM hydrogels exhibited significantly higher tensile properties than those of the Wood/PAM hydrogel and were further assembled into conductive devices for sensor applications. We believe that this UV grafting strategy may facilitate the development of strong wood-based composites with interesting features.