Evidence suggests city grouping is an important way to implement urbanization in China. However, the Chengdu-Chongqing Economic Circle (CCEC) is a typical dual-core structure, and the development level of each city is different. If we do not focus on the key directions for urban development, it will not be conducive to the new-type urbanization process. Therefore, we use spatial analysis techniques and geographic big data sets to construct an approach for urban system layout optimization from a global perspective. It mainly includes urban extended trend analysis based on night light, multi-modal traffic network analysis, and spatial economic density analysis using Open Street Map (OSM) and Point of Interest (POI) data. The research results show the following interesting findings. Firstly, the historical relationship of cities has a significant impact on city grouping, and efficient transportation connections and prosperous enterprise distribution are key conditions for urban grouping during the acceleration period of urbanization. Secondly, the development of urban grouping should break through administrative restrictions and achieve a moderate separation of administrative divisions and economic divisions. It is beneficial to the rapid growth of the city group and the improvement of the internal structure. Thirdly, the urban group of Southern Sichuan and Western Chongqing (SSWC) is the region with the most potential for growth in CCEC. The urban expansion index (UEI) of the Yibin-Luzhou area is 2.16, and the spatial economic density has increased by 130/km2 in the past decade. Providing flexible development authority and focus on the construction of the Yibin-Luzhou Urban Belt along the Yangtze River is an important way to integrate southern Sichuan. Moreover, we found the UEI has a good universality and it can be used for studying urban expansion trends and city relationships in rapidly developing regions, especially in metropolitan areas or urban agglomeration.