Coal remains a primary fuel for power generation. Herein we present time-of-flight secondary ion mass spectra (ToF-SIMS data) taken with a Ga primary ion beam from ca. 30 coal specimens. These commercially different coal specimens were obtained from coal mining companies and/or power plants. They represent all major coal types used in power generation (bituminous coals, subbituminous coals, and lignites), and include low-rank materials (lignites and subbituminous coals), which are represented as a minor portion of the data. Often, inorganic ions (Na+, Al+, Si+, and K+) are pronounced in the spectra, overshadowing peaks from organic moieties. This reflects the high sensitivity of SIMS under our analysis conditions for these inorganic species. These results, including a previous, published chemometrics analysis of this data (L. Pei, G. Jiang, B. J. Tyler, L. L. Baxter, and M. R. Linford, Energy & Fuels 2008, 22, 1059), suggest that ToF-SIMS can be a useful method for coal analysis.