Information leakage and counterfeiting are serious worldwide issues that tremendously impact legitimate businesses and human life. Inspired by the Noctiluca scintillans, a new fluorescence‐afterglow dual‐modal information encryption enabled by precisely coordination‐modulated ultralong organic phosphorescence (UOP) is presented. Strikingly, the optical properties including fluorescence, lifetime and intensity of UOP can be precisely modulated on‐demand through energy transfer by lanthanide (Ln III) coordination, which enables information camouflage by similar Ln III luminescence to provide misleading information along with data decryption in the form of mutual afterglow. Moreover, the important data can be encrypted in a spatial‐time‐resolved way by programmatically coding information with afterglow gradients, yielding greatly improved security for verifying the authenticity. This study provides a new avenue to precisely modulate the optical properties of UOP materials and broadens the scope of optical materials for innovative information encryption and anticounterfeiting applications.
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