The present report deals with the synthesis of isowillardiine (II) and the polyoxin skeleton which have the α-aminouracil structure in common, by the four-component (aldehyde, isocyanide, amine, and organic oxyacid) condensation (Ugi reaction). This reaction permited us to synthesize the above structure (in their protected forms) in one step starting from the corresponding aldehyde. Removal of the protecting group in VIII under conditions of 9N HCl-48 hr afforded isowillardiine, whereas many attempts at complete removal of the protection to XVI is not rewarding, yet.