In this work, lanthanide oxysulfide/oxysulfate compounds, denominated as an oxygen storage and release system, have been synthesized from the anode electrodes of spent Ni-MH batteries. The rare earth metals have recovered by means of chemical precipitation as a mixture of La2(SO4)3, Ce2(SO4)3, and Nd2(SO4)3. The synthesis of (La·Nd)O2S·CeO2 have been carried out by subjecting a mixture of La2(SO4)3, Ce2(SO4)3, and Nd2(SO4)3 to a heat treatment in a reducing atmosphere up to 1000 °C. The (La·Nd)O2SO4·CeO2 compounds have been obtained after thermal treatment of (La·Nd)O2S·CeO2 in a synthetic air atmosphere. The oxysulfide/oxysulfate compounds have been subjected to thermal cycles, respectively, in synthetic air as well as in an N2–CO atmosphere. The thermogravimetric plot (TG) for (La·Nd)2O2S·CeO2 shows a mass gain of 14.98% w/w in a temperature range of 300–550 °C, which is due to the oxidation of (La·Nd)2O2S·CeO2 to (La·Nd)2O2SO4CeO2, where 2 mol of O2 are added. Likewise, in the (La·Nd)2O2SO4CeO2 thermogravimetric plot, a mass loss of 17.16% w/w is observed in the range of 500–750 °C. This loss of mass can be associated with output of 2 mol of O2 forming again the (La·Nd)2O2S·CeO2. The transformation of the (La·Nd)2·O2S·CeO2 to (La·Nd)2O2SO4CeO2 causes an increase in the macropores.