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The novel α-Keggin heteropolyanion supramolecular compound based on organic ammonium and 18-crown-6,[(p-ClANH3)·(18-crown-6)]3·(PMo12O40)·(CH3CN)(1),has been synthesized and characterized by single crystal X-ray diffraction,elemental analysis,IR,UV–vis,PXRD and 1H NMR(p-ClANH2 = p-chloroaniline).The rotator–stator assembly,[(p-ClANH3)·(18-crown-6)]+,was formed through dipolar donor–acceptor attractions,in which the guest p-ClANH3+cation was projected towards the host 18-crown-6 cavity by strong N-H…O18-crown-6H-bonds.The extensive and effective intermolecular hydrogen bonds,among/between organic rotator–stator assemblies and α-Keggin(PMo12O40)3? anion clusters,connected the structural units into a 3D supramolecular functional architecture.In addition,the thermal analysis(TGA and DSC)and luminescent properties were investigated.