Huperzine A, huperzine B, huperzine U and lycoposerramine R are congeners isolated from the Chinese herbal Huperzia serrata (=Lycopodium serratum) in minute amounts.Notably, huperzine A (1), the most significant Lycopodium alkaloid, has aroused tremendous interests due to its nootropic effects.By employing palladium-catalyzed coupling reactions along with a traceless stereocontrol strategy, so far the most efficient asymmetric total synthesis of huperzine A has been achieved.[1] This synthetic strategy, coupled with key transformations including olefin isomerization and Wagner-Meerwein rearrangement, could be successfully extended to the syntheses of relevant Lycopodium alkaloids, such as huperzine B, huperzine U, and lycoposerramine R.