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The hydrotalcite-like compound having ruthenium ions, cobalt ions, and iron ions in the Brucite layer and CO3 anions in the interlayer (Ru-Co-Fe-CO3 HTLC) was found to be effective heterogeneous catalyst for the solvent-free oxidative coupling of 2-naphthols in aerobic conditions. The catalyst could be easily recovered and reused repeatedly for the reaction.