The distribution of nitrogen (N) was determined on 1238 surface sediment samples (0–3 cm) and 24 cores from Lakes Superior, Huron, St. Clair, Erie, and Ontario. The concentration of N was greatest in the depositional basins of the lakes. The N concentrations decreased sharply from high values at the sediment–water interface to uniformly lower N values at the base of the cores. The surface enrichment was related to increased inputs of N to the lakes since settlement of the region in the order: Lake Ontario > Lake Erie Lake Superior > Lake Huron > Georgian Bay.The organic carbon: total nitrogen (C/N) ratios averaged 10.2 in the surface sediments with a range of 5.1 to 66.0. The lowest ratios were found in the depositional basins, with the exception of Lake St. Clair. The magnitude of the C/N ratios was related to the source of the organic matter. Plankton, which are the main source of Org-N in the lakes, accounted for C/N ratios between 7 and 9. Dilution of the modern sediment with organic matter from glacial deposits yielded the higher ratios and low Org-C contents in the nondepositional zones. The high C/N ratios and Org-C contents in Lake St. Clair were believed to be due to a large component of macrophytes in the inputs of organic matter to the lake sediments.