Persistent luminescence has attracted great attention due to the unique applications in molecular imaging, photodynamic therapy, and information storage, among many others. However, tuning the dynamic persistent luminescence through molecular design and materials engineering remains a challenge. In this work, the first example of excitation-dependent persistent luminescence in a reverse mode for smart optical materials through tailoring the excited-state proton transfer process of metal cytosine halide hybrids is reported. This approach enables ultralong phosphorescence and thermally activated delayed fluorescence emission colors highly tuned by modulation of excitation wavelength, time evolution, and temperature, which realize multi-mode dynamic color adjustment from green to blue or cyan to yellow-green. At the single crystal level, the 2D excitation/space/time-resolved optical waveguides with triple color conversion have been constructed on the organic-metal halide microsheets, which represent a new strategy for multi-dimensional information encryption and optical logic gate applications.