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Developing dynamic color‐tunable ultra‐long room temperature phosphorescence (URTP) polymers with afterglow of over 1 s, photo‐chromism, and multi‐stimuli response for practical anti‐counterfeiting and information security applications is attractive but very challenging. Herein, by doping multicolor phosphorescence pyridinium bromide L block or viologen‐based photo‐chromic V block into polyvinyl alcohol matrixes, the water‐stimuli‐responsive color‐tunable URTP polymer films with afterglow of up to 8 s and the reversible viologen‐based photochromic polymer films have been developed. More significantly, a series of dynamic color‐tunable URTP polymer films with ultra‐long afterglow of over 6 s, photo‐chromism, and water‐stimuli response have been successfully exploited by integrating L and V blocks into one polymer system. Mechanistic investigations have revealed that their photo‐chromism mainly comes from the photo‐generated viologen free radicals. Furthermore, their dynamic multilevel anti‐counterfeiting applications have been demonstrated. These results pave the way to develop smarter multifunctional URTP materials for anti‐counterfeiting and optical sensing. [ABSTRACT FROM AUTHOR]