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The relationship between China’s urbanization and economic development (RCUED) is an important concern nationwide. As important actors in regional strategy and policy, county-level regions have played an increasingly significant role in the development of China’s social economy. However, the existing research on the RCUED lacks the fine depiction of the county-level administrative units. Using 2000 and 2010 census data and the statistical analysis method, we uncovered the evolution characteristics of China’s urbanization and economic development and conducted a quantitative identification for the RCUED with improved methods using the quadrant map approach. In addition, we investigated the spatial correlation effect of the RCUED using the spatial autocorrelation analysis method. The results were as follows: 1) In general, a high degree of matching exists between China’s urbanization and economic development at the county level at the significance level of 0.01. The correlation coefficients between China’s urbanization and economic development in 2000 and 2010 were 0.608 and 0.603, respectively. 2) A significant regional difference exists in the RCUED at the county level. Based on a comparative analysis of 2276 county units in China in the two years, we found that county units can be categorized as under-urbanized, basic coordination and over-urbanized in various areas. No situation was observed where urbanization seriously lagged behind the economic development level, so the levels of urbanization and economic development appear to be basically coordinated, and the coordination state may be gradually optimized over time. 3) Over time, the spatial dependency of the RCUED has weakened and the spatial heterogeneity has increased. Northeast China has always been an area characterized by over-urbanization. The number of county units classified as under-urbanized has begun to decline in eastern coastal urban agglomeration areas, while counties rich in resources have transformed from having point-shaped over-urbanization to plane-shaped under-urbanization along the northern border, and the number of over-urbanized county units has increased in the middle reaches of the Yangtze River. 4) ‘Lag-lag’ type and ‘advance-advance’ type accounted for 68% of all counties in China, and these counties were shown to have obvious spatial differentiation characteristics.