Stable symbiotic starter cultures were created using selected strains of Lactobacillus delbrueckii subsp. bulgaricus and Streptococcus salivarius subsp. thermophilus with antimicrobial activity against pathogens and necessary antibiotic sensitivity, growth kinetic parameters, and metabolic profiles. The volatile compound profiles of the obtained starter cultures were determined and their specificity was proven depending on the ratio of monocultures in each combination. The influence of the freeze-drying process on the starter cultures in relation to the production of aromatic components was investigated and it was demonstrated that this process had a significant effect on the content of the aroma-forming substances in the fermented milk. However, the influence of the pre-cooling process and crude fat content from 1.5 to 3.0% did not notably affect the levels of volatile compounds synthesized by the selected starter cultures. Comprehensive data for all volatile aromatic metabolites in the fermented milk were also obtained. These designed symbiotic starter cultures can be used to produce traditional Bulgarian yogurt with increased functional and probiotic properties.