Based on China’s provincial panel data from 2006 to 2019, this paper constructs an evaluation system for the high-quality development of manufacturing industry from five aspects: economic benefits, technological innovation, green development, informatization level and high-end development, and empirically tests the impact of human capital structure on the high-quality development of manufacturing industry. It is found that the optimization of human capital structure can promote the high-quality development of manufacturing industry, and the results are still valid through a series of robustness and endogenous tests; Quantile regression shows that with the improvement of high-quality development level of manufacturing industry, human capital structure plays a stronger role in promoting it; Mechanism analysis shows that human capital structure mainly promotes the high-quality development of manufacturing industry by promoting the technological progress of manufacturing industry, the transformation and upgrading of manufacturing industry and the agglomeration of producer services. Therefore, we should further implement the strategy of strengthening the country with talents, increase R＆D investment, focus on the development of high-tech industries, guide the agglomeration of producer services, in order to boost the high-quality development of manufacturing industry.