The full isotopic pattern for a compound was comprised of the fine and coarse isotopic patterns, excluding duplicate isotopologues from the coarse isotopic pattern that had a mass difference of ≤ than 0.003 Da with any of the other isotopologues, which is the typical mass error observed in LC-HRMS experiments. In this manuscript, a monoisotopic parent ion with one of its isotopologues is referred to as an mono-iso pair. For example, if a monoiso-topic parent ion has 5 theoretical isotopologues, 5 mono-iso pairs are obtained. In total, 2 691 244 mono-iso pairs were generated, which were employed for training (85% of the mono-iso pairs) and testing (15% of the mono-iso pairs) of the probabilistic isotopologue classification model (available on figshare).