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As a derivative of GeTe and MnTe, GeMnTe2 exhibits a cubic structure with no phase transition. Compared to GeTe, it is considerably cheaper and has a significantly high carrier concentration compared to MnTe, making it an excellent thermoelectric (TE) material with promising applications. Herein, a charge‐balanced vacancy engineering strategy is employed, resulting in a significant improvement in the power factor of GeMnTe2. Furthermore, the density functional theory calculation shows that the doping of Bi and the absence of Ge synergically increase the density of states near the Fermi level. Power factors of ≈13.7 μW cm−1 K−2 are achieved at 8% Bi content, a 22% improvement compared to the undoped system, while a final maximum ZT value of about 1.12 and an average ZT value of 0.72 are achieved. This indicates that charge‐balance vacancy engineering is an effective optimization method for the GeMnTe2 system, which can effectively improve the TE performance.