The compounds 2,3-diacetyl, acetoin, hexanoic acid, and isobutyric acid are key aroma contributors significantly affecting consumer preference for Gouda cheese. However, the interaction mechanisms among these aroma compounds and the influence of taste substances on their perception remain unclear. In this study, the olfactory thresholds of these aroma compounds were first determined using systematic analysis based on flavoromics. The interactions between these key aroma compounds and the effects of taste substances on their perception in Gouda cheese were then investigated using S-curve, σ-τ plot, and aroma intensity methods. The thresholds for 2,3-diacetyl, acetoin, hexanoic acid, and isobutyric acid were found to be 0.203 mg/kg, 1.046 mg/kg, 0.673 mg/kg, and 2.710 mg/kg, respectively, in a simulated Gouda cheese matrix. Interaction studies revealed synergistic effects between 2,3-diacetyl and acetoin, as well as between hexanoic acid and isobutyric acid. Additionally, the aroma-taste sensory interaction study indicated that the enhancement of 2,3-diacetyl and acetoin aromas was most pronounced at sodium chloride concentrations of 0.95 g/100 g or 1.50 g/100 g and sucrose concentrations of 10.00 g/100 g or 15.85 g/100 g in the Gouda cheese matrix. These findings provide theoretical support and practical references for improving the aroma quality of Gouda cheese.