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• A MOF based on electron-deficient naphthalene diimide dye is prepared. • The anion–π interactions between two-dimensional network and W6O192– is observed. • Complex 1 exhibits eye-detectable fast-responsive reversible photochromism and photoresponsive luminescence. • Photoinduced electron-transfer produces NDI radicals and W5+ species. Metal-organic frameworks that contain photoactive organic ligands or photoactive inorganic components are an emerging class of multifunctional hybrid materials that in recent years has gradually become an ideal platform for building photochromic complexes. In this paper, a metal-organic framework based on naphthalene diimide (NDI) ligand with Lindqvist-type W 6 O 19 2– polyanions, [Ce 2 (BINDI) (DMF) 8 ]·[W 6 O 19 ] (1), (H 4 BINDI = N, N '-bis(5-isophthalic acid)-1,4,5,8-naphthalene diimide) was synthesized and systematically characterized. It displays a cationic two-dimensional grid coordination network, featuring anion–π interactions between W 6 O 19 2– and expanded π–electron deficient naphthalene diimide (NDI) moieties. Moreover, because of the presence of electron-deficient NDI moieties and photoactive W 6 O 19 2–, this complex exhibits fast responsive reversible photochromism and photoresponsive tunable luminescence. UV–Vis, IR, PXRD, EPR, and XPS spectral studies indicate that the obviously photochromic phenomenon of complex 1 is derived from photoinduced electron-transfer form NDI radicals and W5+ species. [Display omitted]. [ABSTRACT FROM AUTHOR]