The series La2 − x Sr x NiO4 (x = 0.0, 0.05, 0.15, 0.25, 0.35, and 1.0) was tested for functionality as electrode materials for direct electrochemical reduction of NO. The materials were tested using cyclic voltammetry in 1% NO and 10% O2 in Ar on a cone-shaped electrode. The best materials for the electrochemical reduction of NO are La2NiO4 and LaSrNiO4, which have current densities for NO reduction 1.82 and 7.09 times higher, respectively, than for O2 at 400 °C. Increasing the temperature decreased the ability to reduce NO before O2 while the activity increased. The adsorbed species during direct decomposition was attempted, clarified using X-ray absorption near-edge structure experiments and thermogravimetry, but no conclusive results were obtained.