Due to the limitation of 2D spatial resolution, traditional optical information storage technologies, such as optical discs, digital video discs, or Blu-ray discs, are facing increasing challenges. Recently, the fourth generation of ultracapacity optical data storage systems, like far-field super-resolution recording technology [4,5] and multiplexing technology, [6] has come into being. However, owing to the lack of suitable optical storage media, practical applications are still not possible. Herein, the study of new advanced optical materials is of great significance for application of optical information storage.As a potential optical information storage media, electron-trapping materials have attracted considerable attention, since Lindmayer disclosed a 3D optical memory system by utilizing electron-trapping materials in 1986. [7][8][9] When exposed to X-rays, ultraviolet (UV), or visible light, the data can be recorded by arresting the charge carriers in traps. Meanwhile, when stimulated by high-temperature or low-energy laser, data can be read out by releasing the captured charge carriers. Obviously, trap levels play an important role in electron-trapping materials toward optical information storage application. However, most materials with data stored in shallow traps are susceptible to thermal disturbance at room temperature, which greatly hinders its Optical information storage (OIS) is considered as one of the most promising data storage methods due to unique advantages of high security, long life, and low-energy consumption. Combination of optically stimulated luminescence of electron-trapping materials (ETMs) and advanced optical technology has been proved to be a feasible approach to break through physical limitations of traditional storage technology. However, inorganic ETMs are limited to laboratory research, and have not realized the submicron recording point of "microscopic" analog optical storage so far. In this work, an exemplary application of OIS employing inorganic ETMs by a custom-built optical system has been realized for the first time. Multidimensional triple traps are tailored through co-doping of selective rare-earth ions Tb 3+ into Pr 3+ -activated Y 2 GeO 5 . Furthermore, first principles calculations, combined with X-ray photoelectron spectroscopy and low-temperature electron spin resonance spectra, reveal the nature of trap levels. Remarkably, a {10 × 10} array of information points is automatically recorded in a bit-by-bit mode by a 515 nm femtosecond laser, then decoded by linear continuous scanning, and the emission spectrum between each two information points is detected to realize "0" and "1" in binary information. Hopefully, the present work can push forward practical application of inorganic ETMs in high-density and super-speed OIS.