Pycnanthus angolensis has wide application in ethnomedicine and is thus a rich source of medicinally important natural products. The leaf methanolic extract of Pycnanthus angolensis was investigated with the aim of isolating and elucidating the structures of the phytochemical constituents of the plant extract. Isolation and purification of pure compounds was achieved using standard chromatographic techniques. Spectroscopic techniques were used in structural elucidation of new compounds. Two new lignan-lactones, Pycnanolide A and B, were obtained along with four other compounds. The four compounds were identified as β-sitosterol, stigmasterol, phytol and hexadecanoic acid, of which the latter two are encountered for the first time in the plant. Pycnanolide A and B were characterized as (8α, 7'α, 8'β)-3, 4: 3', 4' bis (methylenedioxy) lignan-9, 7'-olide and (8β, 7'β, 8'β)-3, 4: 3',4' bis (methylenedioxy) lignan-9, 7'-olide, respectively. This study helped to characterize the structure of two new lignans-lactones which could form the basis of chemical synthesis and may provide the nucleus for development of new drugs.