Nature Communications, Published online: 12 June 2026; doi:10.1038/s41467-026-74370-9 Direct asymmetric α-C conjugate addition of aminomethylphosphonate to α,β-unsaturated ketones is an intriguing strategy to make bioactive chiral phosphonic 1-pyrrolines. Here, the authors present a direct enantioselective α-C conjugate addition of NH2-unprotected aminomethylphosphonate to α,β-unsaturated ketones using an organo-organo double activation strategy.