Inter-city population movement and attractiveness are two crucial representations for their examination. Measurement of coordination and structural optimization within urban integration zones are vital subjects in the context of regional integration. In order to measure the degree of coordination between population flow and attractiveness among cities in urban integration areas, this paper first combines the gravitational force model and the coupling coordination degree model; it then uses the urban integration areas around Wuhan as an example and analyzes the population flow and coordination between Wuhan and the neighboring cities based on the multi-year Unicom signaling data. In a targeted manner, it offers the optimization plan for each city based on the amount of cooperation. The results show that: (1) there is a significant difference between Wuhan and its neighboring cities in terms of population flow intensity, and (2) Wuhan’s urban integration areas’ overall coordination of population flow is unsatisfactory, with 23.08%, 46.15%, and 30.77% of the total number of cities demonstrating high, medium, and low coordination of population flow and urban attractiveness respectively. Based on the degree of flow coordination, four different types of development methods are provided to meet the development needs of various districts: all-around deep and coordinated development, increased flow intensity, increased attraction strength, and increased flow intensity and attraction strength. This research will help advance research on the coordination level of urban integration areas, utilize big data in territorial spatial planning systems, and support strategic decision-making in metropolitan areas.