efficient, safe, and unclonable information encryption techniques to protect everyone's legitimate rights and interests. [1][2][3][4][5] Compared with other traditional techniques, fluorescent encryption supplies more promising security due to good optical adjustability, distinguishability, and coded storage characteristics. [6][7][8][9][10] However, with the emergence of deep forgery technology, traditional mono-mode fluorescent encryption is far from to meet the requirements of practical applications and cannot ensure high-level data information security. To address such concern, it is imperative to construct high-efficiency multimode luminescent encryption materials with diverse optical structures. [11][12][13] The self-assembly of lanthanide iondoped complexes or layered structure doped with organic sensitizers, both are effective structures for the construction of efficient functional luminescent materials. [14][15][16] Layered rare-earth materials possess adjustable physical and chemical performance, and can be readily functionalized via intercalation features to obtain specific properties. [17,18] Layered rare-earth hydroxide RE 2 (OH) 5 X nH 2 O (where RE = rare earth element, X = anion) is a typical rare-earth layered material, composed of alternating positively charged hydroxide cation layers and charged compensation anion layers. [19,20] Because of its advantages of high stability and low toxicity, it Optical encryption provides a significant implementation strategy for information security, which can be ascribed to multichannel, simple operation, and high security. Multiple responsive luminescent material has emerged as an ideal candidate for optical encryption, owing to intelligent responsive ability and unclonable security. Herein, a structural doping strategy is developed in the layer-by-layer self-assembly process to elevate the maneuverability of light-emitting color and mode. By encapsulating lanthanide doped inorganic matrix and layered hydroxide with PMA, the recognizable red-orange fluorescence can be produced in the invisible region, and realizes the conversion of yellow and green fluorescence in visible region. Meanwhile, both excitation source and emission color can be used as distinguishable encryption means, which enables structural doping complex to be multiplexed and encoded with high capacity and complexity. Furthermore, asymmetrically and symmetrically coded flexible labels with specific color sequence are prepared by brushing process, and specific encryption key are set to ensure the nonlinearity of cryptosystem. Through the integration of dual-mode and adjustable light response codes constructed by structural doping strategy, multidimensional high-level information encryption can be realized, which opens up a deep exploration in the field of information security for the application of multifunctional optical properties of light response materials.