Ruddlesden–Popper (RP) transition-metal oxide phases with the general formula A_n+1B_nO_3n+1 are versatile functional materials that can accommodate a large variety of compositions without compromising structural stability. Substitutions at the A and B sites allow for the precise control of functional properties of these materials. This opens wide possibilities for rational design. In particular, some of these materials were demonstrated to be efficient and stable catalysts for electrochemical oxygen evolution reaction (OER)—one of the key processes in fuel cells and water electrolyzers. In this work, RP phases LaSrM¹_1−xM²_xO_4±δ (M¹, M²—Fe, Co, Ni) with unreported stoichiometry are prepared from aqueous solutions of metal nitrates using the ultrasonic spray-pyrolysis (USP) technique. We found that the phase purity of samples synthesized by USP is higher as compared to samples prepared by solid-state synthesis or by precipitation from aqueous solutions followed by calcination, used in previous studies of RP oxides. LaSrFe_0.5Ni_0.5O_4–δ (LSNF) oxides are found to be very active in OER in alkaline solutions, with overpotential 0.27 V at j = 0.1 A cm^–2 of visible electrode surface in a 5 M solution of KOH. This overpotential is on par with the noble-metal-based OER electrocatalysts. Moreover, the catalytic performance of LSNF in OER is found to be stable over the electrolysis time even in the strongly alkaline solution. These two factors let us conduct the water splitting process in more concentrated electrolytes decreasing the energy cost of hydrogen production by water electrolysis.