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Analyzing the relationship between rural settlements and rural population change under different policy scenarios is key in the sustainable development of China’s urban and rural areas. We proposed a framework that comprised the mixed land use structure simulation (MCCA) model and the human–land coupling development model to assess the spatiotemporal dynamic changes in rural settlements and its’ coupling relationship with the rural population in the economically developed region of Deqing, Zhejiang Province. The results showed that rural settlements and urban land increased by 14.36 and 29.07 km2, respectively, over the last 20 years. The expansion of some rural settlements and urban land occurred at the cost of cropland occupation. Rural settlements showed an expansion trend from 2000 to 2020, increasing from 42.69 km2 in 2000 to 57.05 km2 in 2020. In 2035, under the natural development scenario, the cropland protection scenario, and the rural development scenario, rural settlements are projected to show an expansion trend and Wukang and Leidian are the key regions with rural settlement expansion. The distance to Hangzhou, nighttime light data, distance to rivers, and precipitation are important factors influencing the expansion of rural settlements. The coupling relationship between rural settlements and the rural population developed in a coordinated manner from 2000 to 2020. For 2035, under different scenarios, the coupling relationship between rural settlements and the rural population showed different trends. In the rural development scenario, the highest number of towns with coordinated development between rural settlements and the rural population is in Deqing, predominantly with Type I coupling. Overall, an important recommendation from this study is that the sustainable development of regional land use can be promoted by controlling the occupation of cropland for urban and rural construction, balancing rural settlement expansion and rural population growth, and formulating land use policies that are more suitable for rural development.
