Nature Communications, Published online: 19 August 2026; doi:10.1038/s41467-026-76813-9 γ-Tertiary-nitro-α-amino acids are valuable non-canonical amino acids that remain scarcely explored due to challenges in synthetic accessibility. Here, the authors report a pyridoxal-5′-phosphate (PLP)- dependent enzymatic platform that selectively couples O-acetyl-serine and secondary nitroalkanes to yield γ-tertiary-nitro-α-amino acids.