A new class of carbon dot (CD) grafted cellulose hybrid phosphors has been prepared in a facile and fast process. The reddish-orange emissive CDs can be effectively dispersed in cellulose matrices through hydrogen binding, and thus highly efficient orange-emissive CD-based phosphors were successfully obtained with a quantum yield of 44%. Moreover, the affinity of CDs for binding cellulose provides them the feasibility for fluorescence mapping of cellulosic plant cell walls. Several model plant tissues have been employed to investigate the pathway of CDs. Confocal analysis demonstrated that plant tissues can readily absorb CDs from aqueous solutions and bind them with cellulose-rich structures. These studies may open up new avenues for the exploration of CDs in long-wavelength emissive solid-state lighting and plant tissue imaging.