By core-periphery structure analysis and with the syndication investments events from 2000 to 2014 in China as a sample, this paper studies regional cooperation of Chinese urban venture capital networks. Dynamic venture capital urban networks are constructed every 5 years, and the behavior of cities in the Yangtze Economic Zone analyzed. The following results are obtained. First, a network structure featured by “core, sub-core, semi-periphery, periphery” shows a disparity structure among cities besides the significant phenomenon of spatial agglomeration. Second, regional cooperation is unbalanced, and there is widespread cooperation between core and core, and core and sub-core, while cities in semi-periphery and periphery are more willing to cooperate with those in core or subcore. Third, for cities in core, independent venture capitals (IVCs) are most active no matter in the same city or not, and corporate venture capitals (CVCs) are the second. The case study shows that Shanghai, the only city in core, establishes strangest cooperative relations with sub-core in the Yangtze Economic Zone. Most cities in the Yangtze Economic Zone are in semi-periphery and periphery.