Investigation of the 80% ethanol extract of the aerial parts of Psammosilene tunicoide afforded two carboline alkaloids (1–2), a γ-pyrone derivative (3), two p-hydroxy cinamic acid derivatives (4–5), two glycosides (6–7) and six known compounds (8–13). Their structures were established on the basis of spectroscopic analysis (1D-, 2D-NMR, ESI-MS, and HR-ESI-MS). All these compounds were evaluated for cytotoxicity against SMML-7721, A549, HCT116, and MCF-7 cell lines, and for inhibitory activity against NO production in LPS-induced RAW264.7 macrophages. However, only compound 2 had weak cytotoxic activity against the HCT116 cell line at 20μM, while the others are inactive against four human tumor cell lines and only show weak inhibition activity against NO production at 50μM.