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Abstract The Tibetan grassland ecosystems possess significant carbon sink potential and have room for improved carbon sequestration processes. There is a need to uncover more ambitious and coherent solutions (e.g., Nature-based Solutions) to increase carbon sequestration. Here, we investigated the rationale and urgency behind the implementation of Nature-based Solutions on sequestering carbon using literature review and meta-analysis. We also project the changes in terrestrial carbon sink of Tibetan Plateau grassland ecosystems using model simulations with different future emissions scenario. The results show that the Nature-based Solution projects are expected to increase the carbon sink of Tibetan Plateau grassland ecosystems by 15 to 21 tetragrams of carbon by 2060. We defined a conceptual framework of Nature-based Solutions that integrates initiatives for the restoration of degraded grasslands and carbon sequestration. Our framework consists of four stages: theory, identification, practice, and goal. Traditional Tibetan knowledge plays an important role in reframing the proposed Nature-based Solutions framework. We also apply this framework to optimize ecological restoration techniques and projects and to evaluate the annual changes in the carbon sink under different socioeconomic pathway scenarios.