Metal-organic frameworks (MOFs) have been proven promising ultralong room temperature phosphorescence (RTP) materials for anticounterfeit due to their unique optical properties. However, it remains a major challenge to achieve the desired phosphorescent properties due to the limited regulatory methods and indistinct mechanism. Herein, the coordination solvent and second metal ion costrategy is firstly proposed to prepare seven robust heterometallic-organic frameworks (HMOFs) with two configurations, ZnMg/Ca-sol [sol = H