Historically, Cassia species have been demonstrated to possess several biological activities. However, scientific research on Cassia timoriensis and Cassia grandis remains limited. In this study, the aim was to discover new cholinesterase (ChE) inhibitors to alleviate acetylcholine (ACh) depletion in Alzheimer’s disease (AD). Hence, acetylcholinesterase (AChE) and butyrylcholinesterase (BChE) inhibitory potentials, radical scavenging ability, and anti-inflammatory properties of various extracts of C. timoriensis and C. grandis were carried out using Ellman’s assay, DPPH assay, and an albumin denaturation assay, respectively.