Recently CsTlCl 3 and CsTlF 3 perovskites were theoretically predicted to be potential superconductors if they are optimally doped. The synthesis of these two compounds, together with a complete characterization of the samples are reported. CsTlCl 3 is obtained as orange crystals in two different polymorphs: a tetragonal (I4/m) and a cubic (Fm-3m) phase. CsTlF 3 is formed as a light brown powder, also as a double cubic perovskite (Fm-3m). In all three CsTlX 3 phases Tl 1+ and Tl 3+ were located in two different crystallographic positions that accommodate their different bond lengths. In CsTlCl 3 some Tl vacancies are found in the Tl 1+ position. The charge ordering between Tl 1+ and Tl 3+ was confirmed by x-ray absorption and Raman spectroscopy. The Raman spectroscopy of CsTlCl 3 under high pressure (58 GPa) did not indicate any phase transition to a possible single Tl 2+ state. However, the highly insulating material becomes less resistive with increasing high pressure, while undergoing a change in the optical properties, from transparent to deeply opaque red, indicative of a decrease of the band gap. The theoretical design and experimental validation of the existence of CsTlF 3 and CsTlCl 3 cubic perovskites is the necessary first step in confirming the theoretical prediction of superconductivity in these materials.