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The low-grade bauxite in southern Shanxi Province, China is enriched in multiple critical metal elements, including Li, Ga, V, Se, and rare earth elements (REEs), which have reached the standard of comprehensive utilization as independent deposits or associated resources. Even more importantly, identifying the modes of occurrence of these critical elements is essential for designing technologies to extract critical metals from bauxite ores. This study used a combination of direct (X-ray diffraction, scanning electron microscopy–energy dispersive X-ray spectroscopy, and micro-X-ray fluorescence spectrometer), and indirect (size sieving method, float-sink experiment, and correlation analysis) methods to effectively reveal the distribution of critical elements in the different identified mineral phases. The results regarding the low-grade bauxite are as follows: Li was mainly hosted in cookeite as an independent mineral; Ga was mainly associated with diaspore; anatase is the main carrier mineral for V; REEs were present in the low-grade bauxite in multiples modes of occurrence, the most common of which were goyazite, and to a lesser extent, florencite; Se primarily occurs in sulfides. This study contributes to the development and utilization of these essential metal resources in bauxite by providing a useful reference.