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Six new C-20 and one new C-19 quassinoids, named perforalactones F-L (<b>1</b>–<b>7</b>), were isolated from twigs of <i>Harrisonia perforata</i>. Spectroscopic and X-ray crystallographic experiments were conducted to identify their structures. Through oxidative degradation of perforalactone B to perforaqussin A, the biogenetic process from C-25 quassinoid to C-20 via Baeyer–Villiger oxidation was proposed. Furthermore, the study evaluated the anti-Parkinson’s disease potential of these C-20 quassinoids for the first time on 6-OHDA-induced PC12 cells and a <i>Drosophila</i> Parkinson’s disease model of <i>PINK1^B9</i>. Perforalactones G and I (<b>2</b> and <b>4</b>) showed a 10–15% increase in cell viability of the model cells at 50 μM, while compounds <b>2</b> and <b>4</b> (100 μM) significantly improved the climbing ability of <i>PINK1^B9</i> flies and increased the dopamine level in the brains and ATP content in the thoraces of the flies.