This study analyzed the phytochemical composition and functional properties of leaves and green beans from seven Arabica coffee cultivars. The total phenolic and flavonoid contents were measured using spectrophotometric methods, while caffeine, chlorogenic acid (CGA), and mangiferin levels were quantified via High-Performance Liquid Chromatography (HPLC). Volatile compounds were identified using Gas Chromatography–Mass Spectrometry (GC-MS). Antioxidant activity was assessed using 2,2-Diphenyl-1-Picrylhydrazyl (DPPH) and 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS) radical scavenging assays, and anti-inflammatory effects were evaluated by measuring reactive oxygen species (ROS), nitric oxide (NO) levels, and nuclear factor kappa B (NF-κB) activation in lipopolysaccharide (LPS)-stimulated macrophages. The results revealed that coffee leaves had significantly higher levels of total phenols, flavonoids, and CGAs, and exhibited stronger antioxidant activities compared to green beans. Notably, Geisha leaves exhibited the highest concentrations of phenolics and flavonoids, along with potent anti-inflammatory properties. Among green beans, the Marsellesa cultivar exhibited a significant flavonoid content and strong ABTS scavenging and anti-inflammatory effects. GC-MS analysis highlighted distinct volatile compound profiles between leaves and green beans, underscoring the phytochemical diversity among cultivars. Multivariate 3D principal component analysis (PCA) demonstrated clear chemical differentiation between coffee leaves and beans across cultivars, driven by key compounds such as caffeine, CGAs, and pentadecanoic acid. Hierarchical clustering further supported these findings, with dendrograms revealing distinct grouping patterns for leaves and beans, indicating cultivar-specific chemical profiles. These results underscore the significant chemical and functional diversity across Arabica cultivars, positioning coffee leaves as a promising functional alternative to green beans due to their rich phytochemical content and bioactive properties.