Nine undescribed diketopiperazine alkaloids (1-8, 28) and three undescribed purine alkaloids [35, (±)-36, (±)-37], along with twenty-six known compounds, were isolated from the tubers of Pinellia pedatisecta Schott. Their structures were determined by analysis of their 1D and 2D NMR spectra, HRESIMS, DP4+, ECD, and optical rotation data. In addition, the protective effects of all compounds against Aβ