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This study aimed to compare chemical compositions, antioxidant activities, and acetylcholinesterase inhibitory activities of coffee flowers (ACF) and coffee leaves (ACL) with green coffee beans (ACGB) of Coffea Arabica L. The chemical compositions were determined by employing high‐performance liquid chromatography–mass spectroscopy (HPLC–MS) and gas chromatography–mass spectroscopy (GC–MS) techniques. Antioxidant effects of the components were evaluated using DPPH and ABTS radical scavenging assays, and the ferric reducing antioxidant power (FRAP) assay. Their acetylcholinesterase inhibitory activities were also evaluated. The coffee sample extracts contained a total of 214 components identified by HPLC‐MS and belonged to 12 classes (such as nucleotides and amino acids and their derivatives, tannins, flavonoids, alkaloids, benzene, phenylpropanoids, and lipids.), where phenylpropanoids were the dominant component (>30%). The contents of flavonoids, alkaloids, saccharides, and carboxylic acid and its derivatives in ACF and ACL varied significantly (p <.05) compared to similar components in ACGB. Meanwhile, 30 differentially changed chemical compositions (variable importance in projection [VIP] > 1, p <.01 and fold change [FC] > 4, or <0.25), that determine the difference in characteristics, were confirmed in the three coffee samples. Furthermore, among 25 volatile chemical components identified by GC–MS, caffeine, n‐hexadecanoic acid, 2,2′‐methylenebis[6‐(1,1‐dimethylethyl)‐4‐methyl‐phenol], and quinic acid were common in these samples with caffeine being the highest in percentage. In addition, ACL showed the significantly highest (p <.05) DPPH radical scavenging capacity with IC50 value of 0.491 ± 0.148 mg/ml, and acetylcholinesterase inhibitory activity with inhibition ratio 25.18 ± 2.96%, whereas ACF showed the significantly highest (p <.05) ABTS radical scavenging activity with 36.413 ± 1.523 mmol trolox/g Ex. The results suggested that ACL and ACF had potential values as novel foods in the future. [ABSTRACT FROM AUTHOR]