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The significant role of perovskite defect chemistry through A-site doping of strontium titanate with lanthanum for CO 2 electrolysis properties is demonstrated. Here we present a dual strategy of A-site deficiency and promoting adsorption/activation by making use of redox active dopants such as Mn/Cr linked to oxygen vacancies to facilitate CO 2 reduction at perovskite titanate cathode surfaces. Solid oxide electrolysers based on oxygen-excess La 0.2 Sr 0.8 Ti 0.9 Mn(Cr) 0.1 O 3+δ , A-site deficient (La 0.2 Sr 0.8 ) 0.9 Ti 0.9 Mn(Cr) 0.1 O 3−δ and undoped La 0.2 Sr 0.8 Ti 1.0 O 3+δ cathodes are evaluated. In situ infrared spectroscopy reveals that the adsorbed and activated CO 2 adopts an intermediate chemical state between a carbon dioxide molecule and a carbonate ion. The double strategy leads to optimal performance being observed after 100 h of high-temperature operation and 3 redox cycles, suggesting a promising cathode material for CO 2 electrolysis.