Photoluminescence (PL) has been increasingly applied in anticounterfeiting and encryption as counterfeiting becomes more prevalent. However, common luminescent encryption techniques are based on static PL measurements and are easy to counterfeit. In this work, we have developed a thermal vapor deposition (TVD) approach using melem as the unique starting material to synthesize highly homogeneous carbon nitride (CN) thin films featuring unique dynamic PL switching properties. After being irradiated by a white LED, the blue PL intensity of the CN film increases significantly and then fades in darkness, demonstrating excellent recyclability. Experimental results prove that CN films contain cyano groups in the structure, and density functional theory (DFT) calculations indicate that the integration of cyano groups results in traps within the bandgap of CN, suggesting that the dynamic PL switching effect is essentially associated with the fullness of the trap states. We have therefore developed an advanced luminescent device for the secure transmission of encrypted information through controlled illumination. It can be easily read with a portable UV (365 nm) lamp and effectively erased using the white LED, thereby preventing information leakage and showing great potential for many applications.