Livelihoods encompass three primary dimensions: policy security, ability, and assets. Livelihoods is essential for human survival, understanding the state of people’s livelihoods is essential for human well-being and social governance, particularly in agricultural countries whose social and economic systems are strongly influenced by the environment. However, previous assessment frameworks, including sustainable livelihoods, resilient livelihoods, and vulnerable livelihoods, often confuse different dimensions of livelihood indicators. This could impede a comprehensive understanding of the regional shortcomings as well as the policymaking toward sustainable livelihood. Following Carney’s conceptualization of livelihoods and taking "livelihoods" and "livelihood security" as a starting point, this study proposed a novel muti-level and multi-dimensional sustainable livelihood assessment framework, including 16 indicators across three dimensions - policy security (sustainability at the national level), ability (sustainability at the individual level), and assets. On this basis, we comprehensively evaluated the sustainable livelihood of global agricultural countries and proposed policy recommendations. Results show that: (1) the overall sustainable livelihood status of global agricultural countries was good in 2019, whereas significant disparities existed across three dimensions, with an average score of ( 57.72 ±14.68 ) points for policy security, ( 76.67 ± 20.32 ) points for ability, and ( 18.41 ±13.01 ) points for assets; (2) in terms of the progress from 2001 to 2019, the ability dimension was relatively outstanding (average increase of 17.46 points), while the policy and asset dimensions were almost stagnant (an average increase of 0.97 and 1.77 points, respectively); (3) sustainable livelihood status was also significantly different across income levels, with high-income countries such as European countries exhibiting higher scores than other countries ( 65.77 ± 7.70, P < 0.001), while low-income countries such as those in Africa had the lowest scores ( 37.24 ± 9.10, P < 0.001); (4) further analyses suggested that middle-income countries should focus on education to improve their residents’ livelihood abilities, while low-income countries should pay more attention to policymaking by improving public facilities, improving public health, reducing unemployment rate, and providing skill training. Notably, stagnation or regression in the performance of policy dimensions in most African countries may influence the ability and assets development of population, finally strongly impede their sustainable livelihoods, which calls for urgent policy attention. Overall, by separating different livelihood dimensions, this study delves deeper into specific sustainable livelihood challenges faced by countries at varying developmental stages and facilitates tailored policy recommendations, thereby offering novel insights for global sustainable livelihood research.