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Abstract The development of high‐performance individual marking taggants is of great significance. However, the interaction between taggant and skin is not fully understood, and a standard for marking taggants has yet to be realized. To achieve a highly retentive, anti‐interference, and covert individual marking fluorescent taggant, Mn2+‐doped NaYF4:Yb/Er upconversion nanoparticles (UCNPs), are surface‐functionalized with polyethyleneimine (PEI) to remarkably enhance the interaction between the amino groups and skin, and thus to facilitate the surface adhesion and chemical penetration of the taggant. Electrostatic interaction between PEI600‐UCNPs and skin as well as remarkable penetration inside the epidermis is responsible for excellent taggant retention capability, even while faced with robust washing, vigorous wiping, and rubbing for more than 100 cycles. Good anti‐interference capability and reliable marking performance in real cases are ensured by an intrinsic upconversion characteristic with a distinct red luminescent emission under 980 nm excitation. The present methodology is expected to shed light on the design of high‐performance individual marking taggants from the perspective of the underlying interaction between taggant and skin, and to help advance the use of fluorescent taggants for practical application, such as special character tracking.