A series of negative effects of urban development have emerged owing to the imbalance of population, industry, and built-up land spatial agglomeration. This study proposes an integrated coupling coordination index system in sustainable urbanization evaluation based on population, industry, and built-up land, to evaluate the spatial-temporal evolution of coupling and coordination degree in Guangxi from 2005 to 2015. In addition, we adopted the exploratory spatial data analysis method to reveal the spatial pattern of coupling and coordination degree and its impact on sustainable urbanization. Finally, local indicator of spatial association (LISA) analysis was employed to identify the spatial heterogeneity of the coupling and coordination index values. The results, on the one hand, show that the coupling coordination degree of all counties increased yearly, but extremely slowly. The 88 counties in Guangxi are still in a low level of urbanization. On the other hand, a spatial agglomeration effect of urbanization levels is observed in this study. We found that the urbanization development is not independent. In other words, the urbanization level of each county will more or less be affected by its surrounding counties. In conclusion, in China, sustainable urbanization is closely related to the rational allocation of population, industry, and land resources. To promote the sustainable development of urbanization, it is necessary to strength the role of land use control and to rationally allocate these three elements in general.