Due to the focused pursuit of economic growth in the process of the large-scale urban development of China, the phenomena of low land use efficiency and discordance of land use induce unwanted economic, social, and environmental costs. This paper presents a comprehensive study of urban land use efficiency and of the degree of land use coordination of 33 cities in China, using theoretical analysis, data envelopment analysis, principal component analysis, the coordination coefficient method, and four-quadrant analysis. The findings of this study suggest a gradually increasing proportion of land use efficiency from eastern to central and western regions of China, coinciding with China's pattern of socioeconomic development. No correlation was found between high levels of urban land use efficiency and the degree of land use coordination; however, a significant correlation was found between low land use efficiency and low degrees of land use coordination. Rational land use planning and policy design can effectively improve both urban land use efficiency and coordination.