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This article contains a dataset related to the research published in "The potential of the pecan nut cake as an ingredient for the food industry" [1]. A three-component simplex-centroid mixture design coupled with response surface methodology (RSM) was applied to generate statistical models and to analyze the dataset. The method was also applied to evaluate the effect of different solvents (ethanol, water, and acetic acid) on the extraction of bioactive compounds of pecan nut cake (PNC) and its antioxidant activity. Furthermore, simultaneous optimization of the solvent mixture was carried out to predict the optimum point with the best combination of solvents to obtain an extract with enhanced phytochemical composition, as well as high in vitro antioxidant activity. The maximization of total phenolic compounds, condensed tannins, and antioxidant activity of the PNC was predicted by the desirability function. A total of 80 interactions were run to provide the best condition for optimization. The combined use of the different solvents enables a higher recovery of the compounds than their isolated use. This dataset may help other researchers on the application of a mixture design to recover phytochemicals from a broad range of co-products such as defatted meals and other nut cakes, which are sometimes discarded as waste by many industries., (© 2020 The Author(s).)