Two new seco-dibenzylisoquinoline alkaloids, (-)-secojollyanine (1) and (-)-secohomoaromaline (3), together with the known alkaloid (-)-O-methylpunjabine (2), were isolated from the leaves of Anisocycla jollyana by methanol extraction, column chromatography on silica gel and alumina, and preparative thin-layer chromatography (TLC). Their structures and stereochemistry were determined using chemical methods (e.g., HNO3-H2SO4 color reaction, NaBH4 reduction, CH2N2 methylation, KMnO4 oxidation) and spectrometric techniques including electron impact mass spectrometry (EIMS), fast atom bombardment mass spectrometry (FABMS), infrared spectroscopy (IR), proton nuclear magnetic resonance (1H-NMR), and ultraviolet spectroscopy (UV). The "seco" (ring-opened) nature of compounds 1-3 was inferred from their EIMS (base peaks at m/z 365 for 1 and 2, m/z 397 for 3, arising from benzylic cleavage of seco-dibenzylisoquinolines) and IR spectra (1600 and 1650 cm-1, characteristic of tertiary δ-lactam linkages). For (-)-secojollyanine (1), FABMS revealed a molecular ion [MH+] at m/z 609, supporting the formula C36H36N2O7. Its 1H-NMR spectrum exhibited signals for an N-methyl (δ 2.42), a lactam N-methyl (δ 3.08), two methoxy groups (δ 3.84, 3.86), an ArCH2OH group (δ 4.57), and aromatic protons. Structural confirmation came from NaBH4 reduction to (-)-O-methylpunjabine (2), showing 1 differs by replacing an aldehyde with an alcohol; it shares the same configuration as (-)-O-methylpunjabine. For (-)-secohomoaromaline (3), FABMS gave [MH+] at m/z 639 (C37H38N2O8). Its 1H-NMR spectrum included an aldehyde signal (δ 9.78), three methoxy groups (δ 3.87, 3.95×2), and aromatic protons. UV spectroscopy showed bathochromic shifts (Δ ≤ 1 nm) after alkalinization, indicating a phenolic hydroxyl at the 7′-position (confirmed by CH2N2 methylation). Oxidation of homoaromaline (4) to 3 confirmed a "head-to-head" seco-dibenzylisoquinoline structure and 1'S configuration at C1′. The new alkaloids were named (-)-secojollyanine and (-)-secohomoaromaline.