Thermogravimetry in reducing atmospheres was used to study the oxygen Stoichiometry of several Cu‐substituted lanthanum manganates. The oxygen content of the samples at various levels of reduction (to La2O3, MnO, and Cu) was calculated from the gravimetric data. Freeze‐dried samples prepared by firing at 1100°C in O2 and cooling in O2 had the following composition: LaMnO3.13, LaMn0.7Cuo.3O2.96, LaMn0.5Cu0.5O2.93, and LaMn0.3Cu0.762.71. Single‐phase perovskite structure was obtained in all but the last. The lanthanum manganate LaMnO3.13 was reduced to LaMnO3.00, which shows considerable stability. A 50% substitution of Cu for Mn gave LaMn0.5 Cu0.5O2.93, indicating that the ions involved were mostly Mn4+ and Cu2+. This compound could be reduced to LaMng0.5Cu0.5 O2.26 (largely Mn2+ and Cu1+) without destroying the perovskite structure. This reduced phase could be reoxidized to the original oxygen level but subsequent reduction required considerably higher temperatures and was accompanied by the precipitation of Cu‐rich phases. Samples with a Cu:Mn ratio 30:70 and 70:30 were O‐deficient. The compound LaMn0.7 Cuo.3O2.96 reduced to LaMn0.7Cu0.3O2.54, a relatively stable composition. The highly Cu‐rich sample LaMn0.3Cu0.7O2.71 was easily reduced.