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Whole-grain food ingredients enable the most balanced food products to be obtained, thus forming an important part of a healthy and sustainable diet. Wheat and barley grains are a traditional source of food ingredients for breads, breakfasts, drinks, and snacks in Russia. Such foods are suitable for all ages with many health benefits. However, the modern metropolitan citizen consumes large quantities of refined cereal products, thus impoverishing their diet. An alternative in dietary fortification could be sprouted and fermented food ingredients with an increased nutritional value. The present work was carried out to study the effect of a combination of germination with ultrasound treatment and fermentation with a complex starter of cereal crops on antioxidant activity and γ-aminobutyric acid content of food ingredients with the possibility of using them in the matrix of food products. In order to obtain germinated food ingredients, we used crops with the highest yield in the Ural region (Russia): two samples of soft spring wheat (Triticum aestivum L.) and a sample of spring barley grain (Hordeum vulgare L.). Obtaining food ingredients was divided into successive stages: ultrasonic treatment (22 ± 1.25 kHz) was performed by means of changing power and length of time (245 W/L, intensity for 5 min); germination and fermentation used complex starter “Vivo Probio”. The proposed technology of germination with haunting fermentation of cereal crops resulted in food ingredients with a more uniform distribution of granulometric composition, a low proportion of fine particles (4.62–104.60 µm) (p < 0.05) and large particles (418.60–592.00 µm) (p < 0.05). The particle size range (31.11–248.90 μm) (p < 0.05) was predominant. The germination and fermentation process resulted in 26 to 57% (p < 0.05) lower phytic acid content, 35 to 68% (p < 0.05) higher flavonoid content, 31 to 51% (p < 0.05) higher total antioxidant activity, 42.4 to 93.9% (p < 0.05) higher assimilability, and 3.1 to 4.7 times (p < 0.05) higher γ-aminobutyric acid content, which will allow production of food products with pronounced preventive action. The data was analyzed via one-way ANOVA analysis of variance using the free web-based software. The combination of the germination process with ultrasound treatment and subsequent fermentation with a complex starter can be used to support the development of healthful food products with increased GABA and antioxidant activity.