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  1. Abstract The greenhouse gas methane (CH4) contributed to a warm climate that maintained liquid water and sustained Earth’s habitability in the Precambrian despite the faint young sun. The viability of methanogenesis (ME) in ferruginous environments, however, is debated, as iron reduction can potentially outcompete ME as a pathway of organic carbon remineralization (OCR). Here, we document that ME is a dominant OCR process in Brownie Lake, Minnesota (midwestern United States), which is a ferruginous (iron-rich, sulfate-poor) and meromictic (stratified with permanent anoxic bottom waters) system. We report ME accounting for ≥90% and >9% ± 7% of the anaerobic OCR in the water column and sediments, respectively, and an overall particulate organic carbon loading to CH4 conversion efficiency of ≥18% ± 7% in the anoxic zone of Brownie Lake. Our results, along with previous reports from ferruginous systems, suggest that even under low primary productivity in Precambrian oceans, the efficient conversion of organic carbon would have enabled marine CH4 to play a major role in early Earth’s biogeochemical evolution. 
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  2. The dataset is comprised of analyses of sediment cores and sediment trap samples from ferruginous and meromictic Brownie Lake, Minnesota, U.S.A from January 2018 through February 2021. The dataset includes bulk sediment characteristics including water content, grain size, major and minor elements. Voltammetric scans were collected on porewaters and lake waters. Sediment porewaters were analyzed for pH, total alkalinity, ferrous iron, and dissolved sulfur species contents. Sediment samples were maintained under the exclusion of oxygen for analysis by synchrotron-based X-ray absorption spectroscopy. 
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  3. Depth profiles of water column chemical and physical properties were assessed with seasonal-scale frequency from two meromictic lakes in the upper Midwest, U.S.A. from 2015 to 2019. Brownie Lake in Minneapolis, MN and Canyon Lake in the Huron Mountains of MI both contain elevated hypolimnetic dissolved iron (i.e. “ferruginous”). Several parameters were routinely measured with deployable probes at meter or sub-meter resolution at the deepest location in each lake. Water samples were also collected for laboratory analysis. 
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