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This paper aims to analyze the urban human settlements of 21 megacities and supercities from 2011 to 2020 in China and improve urban human settlements planning and management. First, the data envelopment analysis (DEA)–Malmquist–Tobit model is used to conduct a static and dynamic evaluation of the efficiency of urban human settlements and analyze the main factors that affect it. Then, the coupling coordination degree model is utilized to quantitatively evaluate the coupling coordination degree between urban human settlements and high-quality economic development. Finally, the GM (1, 1) model is established to predict each city's average input–output index during the 14th Five-Year Plan period. It is hoped that this paper could promote sustainable urban development. The empirical results are as follows: (1) the technical efficiency (TE) from CRS DEA of human settlements in China's megacities and supercities is low. Management and technology are the shortcomings in the development of urban human settlements; (2) total factor productivity (TFP) has shown negative growth. Technical progress efficiency (TC) is the key to improving the efficiency of urban human settlements; (3) urban infrastructure has the most significant role when promoting the efficiency of urban human settlements; (4) the coupling degree between the efficiency of human settlements and high-quality economic development is mainly high-level coupling. The degree of coordination is gradually rising; and (5) during the 14th Five-Year Plan period, the investment in human settlements in both types of cities will continue to increase. With the continuous expansion of investment, the output will be imbalanced. [ABSTRACT FROM AUTHOR]