Excitation functions for the formation of 204 m Pb, 203Pb, 202 m Pb, 201Pb, 200Pb, 199Pb, 202Tl and 201Tl in the interactions of natural thallium with protons have been measured by the stacked-foil technique within the proton energy range of 8–45 MeV. For the production of both the medically important radioisotopes 201Tl and 203Pb in a high radionuclidic purity, the optimum incident proton energy was found to be 28 MeV and, theoretically, thick target yields of 0.50 mCi μAh −1 and 3.5 mCi μAh −1, respectively, were achieved. The whole-body radiation dose due to the 200Tl contaminant is five times higher than that due to 201Tl. A target system for the production of 201Tl and 203Pb in a high current compact cyclotron is described. Some observations on the radiochemical separation of lead and thallium are discussed. A procedure for the carrier-free separation of 203Pb and 201Tl activities, employing anion-exchange chromatography, as well as methods for the analytical quality control of the final products are described.