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The continuous development of portable devices and new energy vehicles has led to an increasing demand for high‐performance lithium‐ion batteries (LIBs), and anode materials, as a key part of LIBs, are being explored. Germanium‐based anode materials are considered to have good potential for application because of their high theoretical capacity. In this work, a germanium phosphate glass precipitating GeO2 microcrystal was designed and used in LIBs as anode materials for the study. The presence of GeO2 crystals increases the specific surface area and also provides more reaction sites for lithiation reaction, resulting in the capacity of the glass anode. The discharge specific capacity of the germanium‐phosphorus glass anode was as high as 740.9 mAh g−1 after 600 cycles at a current density of 500 mA g−1. Interestingly, the synergistic effect between the glass matrix and the crystals not only increases the cycling capacity but also enhances the cycling stability of the structure. [ABSTRACT FROM AUTHOR]