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Untargeted metabolomics aims to comprehensively profile metabolites as many as possible in biological samples. Recently, ion mobility-mass spectrometry (IM-MS) has emerged as a powerful technology for untargeted metabolomics. The emerging role of IM-MS in untargeted metabolomics enables the separation of metabolite isomers and generation of multidimension data to support the identification of metabolites. In this review, we first introduced the basic principles of IM-MS instruments commonly used for untargeted metabolomics. Then, we demonstrated the application of IM-MS for metabolite separation and identification of both known and unknown metabolites. Finally, we discussed the future developments of IM-MS technology to improve untargeted metabolomics.