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This study aimed to model and optimize a green sustainable extraction method of phenolic compounds from the coffee husk. Response surface methodology (RSM) and artificial neural networks (ANNs) were used to model the impact of extraction variables (temperature, time, acidity, and solid-to-liquid ratio) on the recovery of phenolic compounds. All responses were fitted to the RSM and ANN model, which revealed high estimation capabilities. The main factors affecting phenolic extraction were temperature, followed by solid-to-liquid ratio, and acidity. The optimal extraction conditions were 100 °C, 90 min, 0% citric acid, and 0.02 g coffee husk mL⁻¹. Under these conditions, experimental values for total phenolic compounds, flavonoids, flavanols, proanthocyanidins, phenolic acids, <i>o</i>-diphenols, and in vitro antioxidant capacity matched with predicted ones, therefore, validating the model. The presence of chlorogenic, protocatechuic, caffeic, and gallic acids and kaemferol-3-<i>O</i>-galactoside was confirmed by UPLC-ESI-MS/MS. The phenolic aqueous extracts from the coffee husk could be used as sustainable food ingredients and nutraceutical products.