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A novel host−guest recognition motif based on a water-soluble pillar[7]arene ( WP7) and a 2,7-diazapyrenium salt ( DMDAP) was prepared. According to the integrated results of 1H NMR, 2D NOESY, UV-vis spectroscopy and fluorescence titration experiments, we demonstrated that the molecular recognition of WP7 to DMDAP in water not only has high association constant but also has pH-responsiveness. Subsequently, we took advantage of this molecular recognition motif to fabricate a supra-amphiphile based on WP7 and an amphiphilic 2,7-diazapyrenium derivative DAPAC. Its controllable self-assembly in water was also investigated by means of TEM and DLS techniques. [ABSTRACT FROM AUTHOR]