This data set contains values on the cheilanthane (tricyclic terpenoids) ratios of C22/C21 and C24/23 from Mesoproterozoic to Silurian rocks of global distribution. Lipid extractions were performed following standard protocols. The yield was contamination-controlled via exterior vs. interior comparison of individual peak concentrations. Values were obtained via integration of multiple-reaction-monitoring (MRM) measurements. In comparing our data of cheilanthane ratios to that reported for younger rocks and oils, we noticed consistently lower C24/C23 values in our samples, suggesting a bimodal character of cheilanthane distribution in time. We tentatively attribute this to the rise of a source of oxidatively decarboxylated cheilanthatriol derived from ferns. Fossil cheilanthanes likely represent a composite mixture of various biological sources, whose secular patterns may record more than the Paleozoic rise of terrestrial plants presented here.