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Targeted poverty alleviation is a unique approach adopted in China to help achieve the vision of a moderately prosperous society in all aspects and the “Chinese Dream”. Industrial development as a means of poverty alleviation is an integral part of the “Five-pronged Poverty Alleviation Measures” Project of targeted poverty alleviation, and a critical foundation for other poverty alleviation measures. In this study, a comprehensive evaluation method was used to measure farmers’ livelihood based on the framework of sustainable livelihood. Specifically, the effects of industrial development on farmers’ livelihood capital were estimated by employing the propensity score matching combined with the difference-in-differences (PSM-DID) approach. Findings suggest that industrial development had a significantly positive effect on the livelihood capital of farmers. Industrial development can significantly enhance farmers’ human, social and financial capital, while it cannot significantly affect the natural and physical capital. Industrial development had heterogeneous effects on farmers’ livelihood capital, more efficiently impacting on the non-poor than the poor. The effects on farmers’ livelihood capital varied across regions, with Guizhou experiencing a larger effect than Sichuan. However, the effect was insignificant for farmers in Gansu. To improve farmers’ livelihood capital, it is necessary to take measures to strengthen their human capital, promote the innovation of financial products, and make good use of their social capital; it is also essential to strengthen the support of industrial development to the poor.