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Herein, we report a 2D MOF based on a phosphonato\u2010amino\u2010carboxylate ligand (NaHL), i.\u2009e., [Na<jats:sub>0.33<\/jats:sub>Co(L)(CH<jats:sub>3<\/jats:sub>OH)<jats:sub>2<\/jats:sub>](NO<jats:sub>3<\/jats:sub>)<jats:sub>0.33<\/jats:sub> (<jats:bold>2<\/jats:bold>), which exhibits an unconventional kagom\u00e9 lattice. The formation of this kagom\u00e9 lattice is caused by the selective recognition of the NO<jats:sub>3<\/jats:sub><jats:sup>\u2212<\/jats:sup> anion by the phenolato group of L<jats:sup>2\u2212<\/jats:sup> as evidenced by theoretical calculations. Compound <jats:bold>2<\/jats:bold> can be utilized for the \u03b1\u2010methoxymethylation and aminomethylation of aromatic ketones using methanol as a C1 source. Interestingly, compound <jats:bold>2<\/jats:bold> can be exfoliated in\u2010situ into nanosheets with one\u2010layer thickness under catalytic reaction conditions, which improves the catalytic efficiency. 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