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We propose an innovative way to produce both 225Ac and 227Th, two precious radioisotopes enabling promising targeted alpha therapy, in a natural thorium target bombarded with a 30–90 MeV electron beam. Bremsstrahlung photons in the target are analyzed by MCNP and in-situ photonuclear transmutation of 232Th is evaluated by using the TENDL nuclear data. In the photo-transmutation analysis, 13 nuclides including 229Th and 231Pa are modelled. Special procedures with chemical separations are also proposed to produce pure 225Ac and 227Th in separate streams. In addition, performance of the new approach is compared with conventional methods in terms of the 225Ac and 227Th yields. After a Th target is bombarded with a 500 kW electron beam for a year, yearly 225Ac yield is ~ 8.47 GBq (semi-permanently) and yearly 227Th yield is ~ 48.9 GBq over 50 years, and their yields are at least doubled in a 2-year irradiation. This work will help increase global supply of the two precious isotopes and would invariably help advance TAT-related researches and developments.