A phytochemical investigation on the aerial part of Phyllodium pulchellum led to the isolation of 16 compounds including five flavonoids (1?5), three lignans (6?8), four indole alkaloids (9?12), and four other-type compounds (13?16). Their structures were elucidated by their spectroscopic data analysis. Among them, 12 compounds (1, 2, 4?9, and 11?14) are reported from the genus Phyllodium for the first time, while compound 14 was isolated from the Leguminosae family for the first time and compound 11 was firstly reported in the plant kingdom. The chemotaxonomic significance of these compounds was also summarized.