715 green coffee samples were gathered by Almacafé S.A. (Bogotá, Colombia) between 2012 and 2014 from 27 different countries and analyzed at the Nuclear Magnetic Resonance (NMR) laboratory at Universidad del Valle (Cali, Colombia). Over 1000 methanolic coffee extracts were prepared and a total of 4563 spectra were acquired in fully automatic mode using a 400MHz NMR spectrometer (Bruker Biospin, Germany). The dataset spans the variance that could be expected for an industrial application of origin monitoring, including samples from different harvest time, collected over several years and processed by at least two distinct operators. The resulting 1D and 2D spectra can be used to develop and evaluate feature extraction methods, multivariate algorithms and automation monitoring techniques, as a dataset for teaching, or as a reference for new studies on similar samples and approach.