The fast‐growing amount of data that is produced every year creates an urgent need for ultracapacity storage media. However, 2D spatial resolution in the conventional optical data storage media has almost reached the limit. Further enlargement of storage capacity may rely on the development of the next‐generation data storage materials containing multiplexed information dimensions. Herein, a series of novel deep‐trap persistent luminescence materials (Sr1‐xBax)Si2O2N2:Eu/Yb,Dy with multicolor emissions in the whole visible region is developed and demonstrated a bit‐by‐bit optical data storage and readout strategy based on photon trapping and detrapping processes in these materials. Optical data can be handily encoded on a flexible film by a commercially available 405 nm laser and decoded by heating or by 980 nm laser scanning. The decoded information contains tunable spectral characteristics, which allows for the emission–intensity–multiplexing or emission–wavelength–multiplexing. The storage and readout strategy not only shows a great promise in the application of multidimensional rewritable optical data storage, but also opens new opportunities for advanced display technology and information security system. A bit‐by‐bit optical data storage and readout strategy based on photon trapping and detrapping processes in deep‐trap persistent luminescence materials is demonstrated in this study. The readout information contains tunable spectral characteristics, allowing for the emission–intensity–multiplexing or emission–wavelength–multiplexing, which may greatly enlarge the storage capacity in multidimensional data storage systems.