This paper reports the catalytic formation of cyanate anion (NCO⁻) from dinitrogen under ambient conditions. A molybdenum-carbamate complex with a PNP-pincer ligand is synthesized and its interconversion with a molybdenum-nitride complex is demonstrated. Samarium diiodide (SmI₂) acts as a reductant, promoting NCO⁻ formation. A two-step synthetic cycle for NCO⁻ from dinitrogen is established, leading to catalytic synthesis under ambient conditions.