We report a simple and effective route to fabricate branched hierarchical flower-like nanostructures of ZnO on natural cotton cellulose fiber by combining electrospinning and the low-temperature hydrothermal growth technique. First, natural cotton cellulose nanofibers were prepared by electrospinning cotton cellulose /LiCl/DMAc solution. The electrospun cotton cellulose nanofibers served as flexible substrate, on which the branched, highly uniform, and dense flower-like ZnO were hydrothermally grown. The as-prepared cotton cellulose/ZnO nanocomposite fibers were characterized by SEM, HRTEM, EDS, TG; and UV-vis spectrophotometry. The modified cotton cellulose nanocomposite fibers were not only exhibiting dispersed uniformly, but also rendered excellent protection against UV radiation because of the incorporation of flower-like ZnO nanostructures. Therefore, the as-prepared nanocomposite fibers demonstrate a significant performance in ultraviolet protection and provide a potential application for ultraviolet detection.