An investigation of the indole alkaloids of Haplophyton crooksii has resulted in the identification of two new alkaloids, 10-methoxy-N1-methylpericyclivine (1) and 16-decarbomethoxyvinervinine (2), and 13 known alkaloids (crooksiine, yohimbine, β-yohimbine, crooksidine, decarbomethoxytetrahydrosecodine, akuammicine, tubotaiwine, lanceomigine, lanceomigine N-oxide, haplophytine, cimicine, cimicidine, and akuammidine) as major alkaloids of this shrub. The authors previously reported the isolation of crooksiine, yohimbine, β-yohimbine, crooksidine, and decarbomethoxytetrahydrosecodine from H. crooksii. In addition to these, 10 more indole alkaloids were isolated and identified, including the two new ones and eight known ones (akuammicine, tubotaiwine, lanceomigine, lanceomigine N-oxide, haplophytine, cimicine, cimicidine, and akuammidine). Of the 15 isolated alkaloids, 1 and 2 are new. All of the isolated alkaloids showed significant in vitro inhibition of acetylcholinesterase activity.