Abstract Efficient conversion of aldoximes and primary amides into nitriles by employing cyclopropenone as an organocatalyst is reported. The reaction proceeds smoothly under mild conditions with 5 mol-% catalyst loading to afford nitriles in excellent yields (78–94%) in a single operation. This method is equally applicable to both aldoximes and primary amides bearing aromatic, heterocyclic, and aliphatic moieties. The convenient and catalytic ...