A large amount of ink has been spilled to paint the picture of China’s urbanization. However, more research might be done on the connotation of sustainable urbanization in China. On the basis of a literature review, this study is the first to propose the perspective of evaluating the sustainability of urbanization from the five dimensions of urbanization: economic, political, cultural, social, and ecological. Based on the Analytic Hierarchy Process (AHP) method and entropy method, a five-dimensional indicator system was established to evaluate the urbanization quality of 31 provincial regions in China during 2005–2015. Then, the coupling coordination degree model was used to calculate the coupling coordination degree of the five dimensions for each region. Furthermore, Moran’s I index and a local indicators of spatial association (LISA) cluster map were used to measure and describe the spatial disparity. Finally, a factor identification model was used to recognize the weaknesses of each region. This study leads to four major findings. (1) In 2015, only ecological urbanization had a high-quality and balanced development, while the development of cultural urbanization was inadequate and regionally unbalanced. Economic, ecological, and cultural dimensions had a significantly positive global spatial autocorrelation. The local spatial autocorrelation varies with dimension. (2) The quality of comprehensive urbanization increased during 2005–2015, while the regional disparity experienced a reduction. A positive global spatial autocorrelation was shown during 2005–2015. The High-High type in the eastern coastal areas centralized over time, while the Low-Low type in the western areas experienced a decline, and the Low-High type was stabilized in the central areas. Only Chongqing was in the High-Low type in 2015. (3) The increase of coupling coordination degree and decrease of coefficient of variation indicated a favorable situation. The coupling coordination degree also had a positive global spatial autocorrelation during 2005–2015. Both the High-High and Low-Low types experienced an obvious shrink and displacement. The Low-High type expanded and centralized in the central areas, while the High–Low type was in Guangdong in 2005, and in Chongqing in 2015. (4) The highest obstacle degrees of each region were all within the cultural dimension, while the ecological dimension caused the least resistance. The lack of innovation had become the biggest barrier in most regions. Based on the above conclusions, this paper concludes with recommendations for policy makers to advance sustainable urbanization in China. Meanwhile, this study can provide lessons and suggestions for other developing countries in the world.