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In this work, the interactions of methane with rare earth metal oxides are studied by using size-specific infrared-vacuum ultraviolet spectroscopy and quantum chemical calculations. Two distinct configurations of methane adsorption are found in the MO(CH4)n (M = Ce, Y; n = 1\u20133) complexes.\u00a0In the first configuration, the C and H atoms of methane are positioned between a Lewis acid-base pair (M2+\u2013O2\u2212); in the second configuration, one H atom of methane is oriented toward a Lewis basic oxygen anion (O2\u2212). Such adsorption features of methane on cerium and yttrium monoxides are dominantly governed by electrostatic interactions. 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