The stems and barks of Tabernaemontana coronaria were investigated previously and have been found to produce indole alkaloids, terpenoids and sterol. However, there seems to be no report on the chemical constituents of the leaves of this plant. The present chemical investigation of the leaves has resulted in the isolation of coronaridine (1), voacristine (2), tabernaemontanine (3) and dregamine (4) from the basic fraction, and lupeol acetate, α-amyrin acetate, lupeol, α-amyrin and sitosterol from the neutral fraction—successively eluted out from the respective columns. Identity of each compound was established by direct comparison (mmp determination, co-TLC, superimposable IR and similar UV) with respective authentic samples. The alkaloids 1, 3 and 4 were previously found in the stem and bark of this plant. The isolation of voacristine, however, constitutes its first report from this plant. While pharmacological studies have shown voacristine and dregamine to be pharmacologically active, there seems to be no such report to our knowledge on coronaridine and tabernaemontanine.