This study employs radiation grafting technology to attach a silane coupling agent onto cotton fabric, followed by the cross-linking of long-afterglow nanoparticles. This process yields a cotton fabric material with a high-intensity long-afterglow luminescence capacity. Characterization techniques, including total reflection infrared spectroscopy, thermogravimetry, X-ray diffraction, and scanning electron microscopy, were employed to investigate the loading of long-afterglow nanoparticles. Additionally, optical performance characterization was conducted to confirm the excellent optical properties of the material. The findings demonstrate that this material exhibits rapid energy charging and high brightness and can emit light continuously for more than 10 h. In addition, the material exhibits satisfactory cyclic and reprocessing performance, meeting the practical requirements of various applications. Because of its straightforward production process, ready availability of raw materials, and remarkable stability, this material holds promising prospects for use in decoration, emergency response, and other domains. This study also offers novel insights into the development of functional fabrics.