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Here, modular assembly of diverse phosphine\u2010amide ligands, including related axially chiral compounds, is first reported through ruthenium\u2010catalyzed C\u2212H activation of phosphines with isocyanate directed by phosphorus(III) atoms. High reactivity and regioselectivity can be obtained by using a Ru<jats:sub>3<\/jats:sub>(CO)<jats:sub>12<\/jats:sub>catalyst with a mono\u2010N\u2010protected amino acid ligand. This transformation significantly expands the pool of phosphine\u2010amide ligands, some of which have shown excellent efficiency for asymmetric catalysis. More broadly, the discovery constitutes a proof of principle for facile construction of hemilabile ligands directly from the parent monodentate phosphines by C\u2212H activation with ideal atom, step and redox economy. 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