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HSR studies have been one of the most important issues in economic geography, transport economics and policy. However, prior studies give rare attention to its role on the technological innovation collaboration, which become increasing important nowadays. Using co-patent data of the State Intellectual Property Office (SIPO) database from 2000 to 2016, this paper investigates the role of HSR services in cross-city technological innovation collaboration. Empirical results show: 1) the intensity of cross-city technological innovation collaboration activities remains at a low level before the debut of HSR services in China, and the difference on this indicator between cities with and without HSR services is statistically insignificant. With the emergence of HSR network, cross-city innovation collaboration is booming and cities with and without HSR services show distinct trends. 2) HSR services play a significant positive role in stimulating the intensity of cross-city technological innovation collaboration activities of HSR cities. 3) megacities benefit most from the HSR network, and secondary cities also benefit from being connected to megacities by HSR lines. 4) The travel time between city pairs is significantly correlated with the intensity of collaborative innovation activities. Our results suggesting interregional innovation bonds, which implicitly featuring the channel of knowledge flow, are established or strengthened by high-speed transport investments.