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In the strong orange luminescent material of [Pb(bp4mo)Cl2], two different types of octahedra, namely PbCl4N2 and PbCl4O2, are bridged by the N-oxide-4,4′-bipyridine (bp4mo) ligand, while its protonated form, Hbp4mo+, coordinates to Pb2+ center only with the N-oxide group in [Pb(Hbp4mo)2Cl2](NO3)2. Important relationships between structures and luminescence properties are revealed.