Two new C-21 Daphniphyllum alkaloids, longeracinphyllins A (1) and B (2), have been isolated from the leaves of Daphniphyllum longeracemosum. Longeracinphyllin A (1) is a new daphnilongeranin B type alkaloid with a rearranged alpha,beta-unsaturated ketone group, and the structure is supported by X-ray crystal data. Longeracinphyllin B (2) is a new seco-10,17-daphnilongeranin B type alkaloid.