We report a green and efficient method for chemoselective deoxidization of graphene oxide via the ultraviolet irradiation catalyzed with 2,2,6,6-tetramethyl-4-piperidinol. While the sp(2)-hybridized oxygen functional groups are removed after the reduction, the epoxy and hydroxyl groups are retained in the chemoselectively reduced graphene oxide (CrGO). The obtained CrGO nanosheets exhibit the high solubility and excellent electronic stability, which allows for the fabrication of thin film devices through a solution processing. As a proof of concept, a CrGO-based write-once-read-many-times memory device with the desirable stability and long-time operation is fabricated.