Carbon (C) release from thawing permafrost is potentially the largest climate feedback from terrestrial ecosystems. However, the magnitude of this feedback remains highly uncertain, partly due to the limited understanding of how abrupt permafrost thaw (e.g., permafrost collapse) alters soil organic matter (SOM) quality. Here we employed elemental analysis, stable isotope analysis, biomarker and nuclear magnetic resonance techniques to explore changes in soil C concentration and stock as well as SOM quality following permafrost collapse on the Tibetan Plateau. Our results showed that permafrost collapse resulted in a 21% decrease in soil C concentration and a 32% reduction in C stock of the top 15 cm of soil over 16 years. Moreover, permafrost collapse led to a significant decline in SOM quality: the relative abundance of labile SOM fractions (e.g., carbohydrates) decreased, whereas recalcitrant SOM fractions (e.g., suberin-derived compounds) increased 16 years after collapse. By contrast, the relative abundances of labile and recalcitrant compounds showed no significant differences in the control plots along the thaw sequence. These results demonstrate that permafrost collapse and consequent changes in soil environmental conditions could trigger substantial C release on decadal timescales, implying that abrupt thaw may be a dominant mechanism exposing soil C to mineralization.