Concise total syntheses of rac‐ and (+)‐goniomitine were developed. The cyanide‐catalyzed imino‐Stetter reaction of an aldimine, derived from ethyl 2‐aminocinnamate and either rac‐ or (S)‐α,β‐unsaturated aldehyde bearing a δ‐valerolactam at the β‐position, provided rac‐ or (S)‐indole‐3‐acetate carrying an α‐vinyl‐δ‐valerolactam scaffold at the 2‐position, respectively. Subsequent saturation of the vinyl group, followed by treatment with DIBAL‐H, afforded N‐benzyl protected goniomitine. Final debenzylation provided the desired natural product after only three column separations.