Organic room temperature phosphorescence (RTP) from polymers holds significant promise for information encryption and anti‐counterfeiting applications. However, conventional patterning techniques limit the development of advanced RTP encryption, highlighting the need for an efficient method that achieves encryption processes quickly and conveniently. In this study, the UV laser marking machine is applied to create traceless phosphorescent patterns by leveraging the photothermal effect of the laser and the water‐absorbent quenching RTP property of polyacrylamide. A series of biaryl derivative phosphors with low π‐electron numbers are designed to limit UV absorption to below 355 nm, thereby preventing polymer sintering by the UV laser (355 nm). Additionally, two phosphorescent polymers, PB2COOH (phosphorescence lifetime τP = 2.34 s; phosphorescence quantum yield ΦP = 13.59%) and PBN (τP = 1.46 s; ΦP = 20.33%), possessing relatively excellent phosphorescent properties, are obtained. The controllable program and non‐contact processing of the marking machine enable the rapid realization of complex patterns, such as the Twelve Chinese Zodiac Signs, effectively overcoming the constraints of traditional techniques. Based on this laser technology, applications such as dual‐locking QR (quick response) codes, misleading double QR codes, labeling, and other advanced encryption methods are developed.