Long-lived room temperature organic phosphorescence is highly useful in biological imaging, electroluminescent devices, information security, and security protection on account of its unique photophysical process and long-lived luminescence. In recent years, pure organic phosphorescent materials that do not contain rare precious metals have received increasing attention. Carbazole and its derivatives have been used to develop room temperature organic phosphorescent materials. However, the effect of carbazolyl groups on the photophysical properties of pure organic phosphors has rarely been reported. In this work, three cyanuric chloride phosphors (CzDCIT, BiCzDT, and TCzT) modified with different numbers of carbazolyl groups were synthesized. Several characterization techniques were employed to reveal distinct crystal forms of CzDCIT, BiCzDT, and TCzT. The single crystal diffraction of CzDCIT and BiCzDT showed not only different crystal packing modes, but also the formation of internal H-aggregation. These three phosphor powders exhibited dual emissions of blue fluorescence and yellow phosphorescence at room temperature, with luminescence lifetimes of 0.16-0.34 s. Theoretical calculations indicated that different numbers of effective intersystem crossing channels between CzDCIT, BiCzDT, or TCzT were responsible for the luminescence lifetimes. After doping the phosphors into the polymer matrix, they exhibited good persistent phosphorescence and high recoverability in multiple compression-grinding cycles. © 2019 American Chemical Society.