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Cities worldwide are stepping up efforts to reshape their infrastructure to ensure a carbon-neutral and sustainable future, leading to the rapid electrification of transportation systems. The electricity demand of this sector, particularly that of high-speed railways, is increasing. Application of the existing infrastructures of railway stations and available land along rail lines for photovoltaic (PV) electricity generation has the potential to power high-speed bullet trains with renewable energy and supply surplus electricity to surrounding users. In this work, a methodology based on a geographic information system was established to evaluate the PV potential along rail lines and on the roofs of train stations. The Beijing-Shanghai high-speed railway (HSR) was used as a case study. Its total PV potential reached 5.65 GW (of which the station potential accounted for 264 MW, approximately 4.68%, of the total potential), with a lifelong generation capacity of 155 TWh, which corresponds to approximately 12% of the total new installed capacity of China in 2020. Although electricity prices and solar resources differed along the railway line, all PV systems were profitable. Moreover, a comparison between the electricity consumption and generation shows that the PV+HSR system can cover most of the electricity demand of the Beijing-Shanghai HSR without a storage system. This concept can be further expanded to other rail lines and stations. Within the context of global carbon peaks and carbon neutrality, the integration of PV and railway systems should be promoted.