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Species adulteration is a common problem in the coffee trade. Several attempts have been made to differentiate among species. However, finding an applicable methodology that would consider the various aspects of adulteration remains a challenge. This study investigated an ultraviolet–visible (UV-Vis) spectroscopy-based determination of caffeine and chlorogenic acid contents, as well as the applicability of non-targeted near-infrared (NIR) spectroscopy, to discriminate between green coffee beans of the <i>Coffea arabica</i> (Arabica) and <i>Coffea canephora</i> (Robusta) species from Java Island, Indonesia. The discrimination was conducted by measuring the caffeine and chlorogenic acid content in the beans using UV-Vis spectroscopy. The data related to both compounds was processed using linear discriminant analysis (LDA). Information about the diffuse reflectance (log 1/R) spectra of intact beans was determined by NIR spectroscopy and analyzed using multivariate analysis. UV-Vis spectroscopy attained an accuracy of 97% in comparison to NIR spectroscopy’s accuracy by selected wavelengths of LDA (95%). The study suggests that both methods are applicable to discriminate reliably among species.