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Stoichiometric natural gas (CNG) engines are an attractive solution for heavy-duty vehicles considering their inherent advantage in emitting lower CO2 emissions compared to their Diesel counterparts. Additionally, their aftertreatment system can be simpler and less costly as NOx reduction is handled simultaneously with CO/HC oxidation by a Three-Way Catalyst (TWC). The conversion of methane over a TWC shows a complex behavior, significantly different than non-methane hydrocarbons in stoichiometric gasoline engines. Its performance is maximized in a narrow A/F window and is strongly affected by the lean/rich cycling frequency. Experimental and simulation results indicate that lean-mode efficiency is governed by the palladium’s oxidation state while rich conversion is governed by the gradual formation of carbonaceous compounds which temporarily deactivate the active materials.