We present polar ice core organic matter (OM) fluorescence signatures to reconstruct ancient and modern atmospheric compositions and relate OM signals to past ecological changes. OM composition from three Arctic ice cores (Canada and Greenland) was characterized by fluorescence spectroscopy and compared to an Antarctic OM record. Diverse OM was measured in ancient and modern ice in both hemispheres and similarities existed across vast spatiotemporal scales. We determined three OM markers, indicating paleoclimate and modern carbon trends: (i) ‘humic-like’, detected in Holocene ice of more complex and aromatic character, supporting trends of higher plant influences in warmer climates, (ii) monolignol- and non-amino acid-like, describing simple, lignin-like OM precursors ubiquitous in the environment and the microbial degradation products of more complex materials from plants/soils, and (iii) amino acid- and tannin-like, indicating microbial degradation of simple OM chemical species, compared to the other markers. Concentration trends were inferred from fluorescence intensities of individual OM types and related to warmer temperatures. No indicators of freshly produced OM by microbes were detected; signals were interpreted as materials externally produced from the ice and transported to polar regions. This marks the first global comparison of atmospheric reconstructions from OM across vast spatiotemporal scales.