Long-lived afterglow room-temperature phosphorescence (RTP) from natural phenolics has seldom been reported yet this is essential for the development of sustainable afterglow RTP materials. With this research, we have prepared sustainable afterglow RTP materials (GA@SA) with a lifetime of up to � 934.7 ms by embedding gallic acid (GA) within a Ca 2 + -crosslinked sodium alginate (SA) matrix. Theoretical simulations indicate that the restricted carbonyl moieties of the GA and H-type aggregates of GA in a SA matrix promoted the spin orbit coupling (SOC) of GA and induced afterglow emission. Moreover, afterglow RTP emission could be produced by embedding different types of natural phenolics such as, tannic acid, caffeic acid and chlorogenic acid into Ca 2 + -crosslinked networks of SA. As an illustration of potential applications, GA@SA was used to prepare anti-counterfeit afterglow clothing and paper. This work provides an innovative method for the activation of long-lived afterglow RTP from sustainable phenolics.