A short lifetime, low phosphorescence quantum efficiency (PQE), and unstable room-temperature phosphorescence (RTP) in oxidants and solvents are the core problems in the development of carbon dot (CD)-based RTP materials for anticounterfeiting applications. Herein, a series of CDs/Al 2 O 3 nanocomposites with excitation-dependent RTP properties were fabricated by a sol−gel process followed by high-temperature treatment. The crystalline structure and rigid Al−O network of the Al 2 O 3 matrix could readily benefit the stabilization of the triplet excited state of CDs. The Al−O−C interactions between the CDs and Al 2 O 3 favor the facilitation of intersystem crossing (ISC) to effectively populate triplet excitons, which contributes to the RTP with a low energy gap. As a result, an ultralong lifetime of up to 1.4 s (observed by the naked eye for 22 s) and a high PQE of 12.78% were achieved by CDs/Al 2 O 3 -500 and CDs/Al 2 O 3 -300, respectively. The results demonstrated that the oxidants, polar solvents, and strong acids and alkalis almost had no effect on the RTP emission of the CDs/Al 2 O 3 nanocomposites. Taking advantage of the ultralong phosphorescence afterglow, excitation-dependent multicolor RTP emission, and excellent stability, graphics of the Eight Trigrams were present for advanced anticounterfeiting via time-resolved luminescence imaging based on different CDs/Al 2 O 3 nanocomposites.