AbstractTunable full‐color room temperature phosphorescence (RTP) is charming due to its potentials in multiple anticounterfeitings, all‐color displays, and multichannel biomarkers. However, it is a huge challenge to achieve excitation‐dependent continuously adjustable full‐color RTP from a single‐component compound. Herein, two Zn(II)‐based organic coordination polymers are reported, which are the first examples characterized by blue, cyan, green, yellow, orange, and red continuously tunable phosphorescence with decent quantum efficiencies in response to variation of excitation energy at ambient conditions. The unique photoluminescence behavior is induced by the selective formation and decay of multiple triplet excited states, i.e., ligand‐centered 3π–π*, 3(ligand‐to‐ligand charge transfer), 3(halogen‐to‐ligand charge transfer), etc., in the coordination network based on the varying excitations. The population and stabilization of the unusual triplet excitons of Zn(II)‐based organic coordination polymers benefit from heavy atom effect of Br− ions and the restriction of molecular motion by crystallization. Here an insight is contributed for the construction of full‐color RTP materials, and metal‐organic coordination polymers are endowed with fresh features for extensive applications.