In the emerging field of high-capacity information encryption, multicolor, multitemporal, and multimodal luminescence inorganic materials are of great significance. However, conventional inorganic materials lack the flexibility to dynamically adjust the photon transition path, resulting in unicolor luminescence of the sample and reducing the reading and decoding levels. Herein, we elaborately designed the components for constructing dual-phase crystal fields for Eu 2+ in phosphors based on a high temperature solid-state method. Specifically, SrAl 2 O 4 :Eu 2+ crystal with a bright green afterglow and CaAl 2 O 4 :Eu 2+ crystal with a blue afterglow were obtained in phosphors at the same time. As a result, a tunable afterglow behavior from blue to white was achieved due to the 4f 6 5d 1 → 4f 7 transition of Eu 2+ at different crystal field sites. Finally, the color tunable afterglow sample was used to explore the encryption and decryption processes of information, and the results showed that the prepared material has a good anti-counterfeiting performance, which is promising for the development of long persistent luminescent materials.