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Graphical abstract Highlights • Perovskites with Mn and Fe as B cation successfully prepared and tested in STS. • Mixed materials show structural features intermediate between pure Mn and Fe perovskites. • The presence of Fe improves self-reduction and, therefore, the producible H 2. • The presence of Mn improves the oxidation kinetics, lowering typical splitting temperature. • Use of diverse B ions as an effective strategy to manage self-reducibility and splitting activity. Abstract Mixed perovskites, described by the formula La 0.6 Sr 0.4 Mn 1−x Fe x O 3−δ with x ranging from 0 to 1, were prepared and tested as potential catalysts for the solar thermochemical water and carbon dioxide splitting. The increase of iron amount promotes the reduction step according to the trend of the starting reduction temperatures; on the other hand, the reactivity towards H 2 O and CO 2 seems to be fostered by high Mn contents. The highest amounts of oxygen evolved during thermogravimetric analysis and hydrogen produced during splitting tests occur to the sample with x = 1 even if a non-monotonic trend with iron substitution is appreciated. Instead, CO amount progressively decreases by increasing iron content. The results reported in this work indicate that the formulation of bi-functional systems with two active sites, one showing good self-reduction the other good reactivity towards splitting reactions, is the best route to prepare materials with larger intrinsic H 2 and CO productivity as well as lower reduction/oxidation temperature. [ABSTRACT FROM AUTHOR]