A new microporous Zr(W)-based metal organic framework (MOP) containing 4,4',4 '',4'''-(9,9'-spirobi[fluorene]-2,2',7,7'-tetrayl)tetrabenzoic acid (Spirof-MOF) was synthesized, characterized, and size controlled for the adsorption and decomposition of a nerve agent simulant, dimethyl 4-nitrophenylphosphate (DMNP). Spirof-MOF showed a hydrolysis half-life (t(1/2)) of 7.5 min to DMNP, which was confirmed by using in situ P-31 NMR spectroscopy. Additionally, 'size-controlled Spirof-MOFb (similar to 1 mu n) exhibited a half-life of 1.8 min and 99% removal within 18 min for DMNP. The results show that Spirof-MOF is a new active material in removing nerve agent simulants by adsorption and hydrolytic decomposition.