Anticounterfeiting labels based on physical unclonable functions (PUFs), as one of the powerful tools against counterfeiting, are easy to generate but difficult to duplicate due to inherent randomness. Gap-enhanced Raman tags (GERTs) with embedded Raman reporters show strong intensity enhancement and ultra-high photostability suitable for fast and repeated readout of PUF labels. Herein, we demonstrate a PUF label fabricated by drop-casting aqueous GERTs, high-speed read using a confocal Raman system, digitized through coarse-grained coding methods, and authenticated via pixel-by-pixel comparison. A three-dimensional encoding capacity of over 3 × 1015051 can be achieved for the labels composed of ten types of GERTs with a mapping resolution of 2500 pixels and quaternary encoding of Raman intensity levels at each pixel. Authentication experiments have ensured the robustness and security of the PUF system, and the practical viability is demonstrated. Such PUF labels could provide a potential platform to realize unbreakable anticounterfeiting.