LAUSR

SrMoO3 , SrNbO3, and SrVO3 are remarkable highly conducting d1 (V, Nb) or d2 (Mo) perovskite metals with an intrinsically high transparency in the visible. A key scientific question is how the optical properties of these materials can be manipulated to make them suitable for applications as transparent electrodes and in plasmonics. Here, it is shown how 3d/4d cationic substitution in perovskites tailors the relevant materials parameters, i.e., optical transition energy and plasma frequency. With the example of the solid‐state solution SrV1−xMoxO3, it is shown that the absorption and reflection edges can be shifted to the edges of the visible light spectrum, resulting in a material that has the potential to outperform indium tin oxide (ITO) due to its extremely low sheet resistance. An optimum for x = 0.5, where a resistivity of 32 µΩ cm (≈12 Ω sq−1) is paired with a transmittance above 84% in the whole visible spectrum is found. Quantitative comparison between experiments and electronic structure calculations show that the shift of the plasma frequency is governed by the interplay of d‐band filling and electronic correlations. This study advances the knowledge about the peculiar class of highly conducting perovskites toward sustainable transparent conductors and emergent plasmonics.