Organic matter (OM) dynamics determine how much carbon is stored in ecosystems, a service that modulates climate. We synthesized research from across the US Long-Term Ecological Research (LTER) Network to assemble a conceptual model of OM dynamics that is consistent with inter-disciplinary perspectives and emphasizes vulnerability of OM pools to disturbance. Guided by this conceptual model, we identified unanticipated patterns and long-term trends in processing and transport of OM emerging from terrestrial, freshwater, wetland, and marine ecosystems. Cross-ecosystem synthesis combined with a survey of researchers revealed several themes: 1) strong effects of climate change on OM dynamics, 2) surprising patterns in OM storage and dynamics resulting from coupling with nutrients, 3) characteristic and often complex legacies of land use and disturbance, 4) a significant role of OM transport that is often overlooked in terrestrial ecosystems, and 5) prospects for reducing uncertainty in forecasting OM dynamics by incorporating the chemical composition of OM. Cross-fertilization of perspectives and approaches across LTER sites and other research networks can stimulate the comprehensive understanding required to support large-scale characterizations of OM budgets and the role of ecosystems in regulating global climate.