A one‐step synthesis of N‐methyl‐2‐aryl‐4‐quinolone alkaloids is described. These compounds are readily prepared from the reaction of an N‐methylisatoic anhydride with the lithium enolate of an acetophenone. By this method, the reaction of N‐methylisatoic anhydride (5) or 5‐methoxy‐N‐methylisatoic anhydride (7) with acetophenone produces the alkaloids N‐methyl‐2‐phenyl‐4‐quinolone (1) and eduline (2) in 81% and 70% yield, respectively. An analogous reaction of 5 with 3,4‐methylenedioxyacetophenone gives graveoline (3) in 63% yield whereas 7 and α‐methoxyacetophenone affords japonine (4) in 61% yield.