Tamarindus indicaLinn (tamarind, F. Leguminosae) is one of the most widely consumed edible fruits in the world. Phytochemical investigation of tamarind pulpn-butanol fraction yielded one new (+)-pinitol glycoside compound1(25%w/w), and 1D, 2D NMR, and HRESIMS investigation were used to confirm the new compound’s structure. (+)-Pinitol glycoside showed anti-Alzheimer potential that was confirmed in prophylactic and treatment groups by decreasing time for the T-maze test; decreased TAO, brain and serum AChE, MDA, tau protein levels, andβamyloid peptide protein levels; and increasing GPX, SOD levels, and in vivo regression of the neurodegenerative features of Alzheimer’s dementia in an aluminum-intoxicated rat model. The reported molecular targets for human Alzheimer’s disease were then used in a network pharmacology investigation to examine their complex interactions and identify the key targets in the disease pathogenesis. An in silico-based analysis (molecular docking, binding free energy calculation (ΔGBinding), and molecular dynamics simulation) was performed to identify the potential targets for compound1. The findings of this study may lead to the development of dietary supplements for the treatment of Alzheimer’s disease.