Room-temperature phosphorescent (RTP) carbon dots (CDs) have promising applications in bioimaging, anticounterfeiting, and information encryption owing to their long lifetimes and wide Stokes shifts. Numerous researchers are interested in developing highly bright RTP CDs using environmentally friendly and safe synthesis processes (e.g., natural raw materials and zero-pollution production pathways). In this study, we successfully synthesized RTP CDs using a hydrothermal process employing natural vitamins as a raw material, ethylenediamine as a passivator, and boric acid as a phosphorescent enhancer, which is referred to as phosphorescent CD (PCD). The PCDs exhibit both bright blue fluorescence emission and green RTP emission, with a phosphorescence lifetime as long as 293 ms and an excellent green afterglow visible to the naked eye for up to 7.0 s. The total quantum yield is 12.69%. The phosphorescence quantum yield (PQY) is up to 5.15%. Based on the RTP performance, PCDs have been successfully employed for anticounterfeiting and information protection applications. The results of this study provide a green strategy for the scalable synthesis of RTP materials, which is a practical method for the fabrication of RTP materials with high efficiency and long afterglow lifetimes.