Fermentation, a critical post-harvest process, can be strategically manipulated to augment coffee quality. This enhancement is achieved through the activity of microorganisms, which generate metabolites instrumental in the formation of distinct sensory profiles. This study investigated the impact of different fermentation methods on the quality of coffee beverages, specifically utilizing the Catiguá MG2 variety. The experimental setup involved fermenting the coffee in 200 L bioreactors, employing both natural and pulped coffee beans. The fermentation process utilized was self-induced anaerobic fermentation (SIAF), conducted in either a solid-state or submerged medium over a 96 h period. Analytical sampling was conducted initially and at 24 h intervals thereafter to quantify the concentration of sugars, alcohols, and organic acids. Sensory evaluation was performed using the established protocols of the Specialty Coffee Association (SCA). The outcomes of this investigation reveal that fermentation substantially enhances the quality of coffee, with each treatment protocol yielding divergent profiles of acids and alcohols, thereby influencing the sensory characteristics of the resulting beverage. Notably, superior quality beverages were produced from naturally processed coffee subjected to solid-state fermentation for durations exceeding 24 h. These findings underscore the significant influence of fermentation techniques and duration on the sensory attributes and overall quality of coffee.