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Inland waterbodies play an important role in the global carbon cycle, acting both as carbon sources with organic carbon (OC) mineralization and as sinks with OC burial in sediments. Under recent impacts of global warming, anthropogenic land-use change and nutrient supply, however, there is a limited knowledge regarding OC dynamics in sediments of large, deep lakes especially in subtropical alpine regions. Here, we studied the patterns of OC burial and the potential regulating factors using multiple sedimentary proxies and observational records in Lugu Lake (southwest China) over the past ~100 years. Comparisons of 15 sediment cores in different areas of the lake reveal similar temporal trends in OC content and other sediment parameters, indicating coherent patterns of whole-lake sedimentary environmental change dominated by watershed human perturbation. Based on C/N ratios and δ13Corg analyses, the sediment OC has primarily been autochthonous in source. OC accumulation rates (OCAR) increased during 1880–1980, from ~14 to 43 g C m−2 yr−1 in a central core (LGS), mainly resulting from elevated primary production under increased phosphorus input and soil erosion. Subsequently, OCAR decreased considerably to ~15 g C m−2 yr−1, although the phosphorus supply and lake primary productivity remained high. We infer the OCAR decline likely resulted from increased organic matter decomposition and OC mineralization in the water column because of climate warming and lake-water thermal stratification. This phenomenon might mask the positive contribution of primary production to OC burial. Our findings suggest that the commonly observed synergistically positive effects of warming and eutrophication on sediment OC burial may be impaired in deep lakes, which needs further investigations across ecological, climatic and land-use gradients.