The hydroprocessing of gasoline on modified alumina catalysts makes it possible to obtain high-octane products. The implementation and development of the process have largely become possible due to the development of modified alumina catalysts that do not contain noble metals and exhibit special catalytic properties. This article discusses topical issues of petrochemistry, namely the creation of catalysts with improved characteristics for the production of high-octane gasoline with low sulfur content. New catalytic systems based on alumina and other carriers modified with transition metals, lanthanum and phosphorus were synthesized. By physico-chemical methods of analysis TPD of ammonia, TEM and XRD, we studied the acid–base and structural characteristics of the developed catalysts. The activity of the developed catalysts in the studied process of hydrotreating gasoline fractions depends on the structure and condition of the active centers. The process of hydrotreating straight-run gasoline in the presence of synthesized catalysts was carried out on a laboratory flow unit. It was shown that, during the hydrotreating of straight-run gasoline on the NiO-MoO3-La-P-HZSM-HY-Al2O3 catalyst, the octane number in the final product increased to 88.6, and the sulfur content decreased from 0.0088 to 0.001%. It was found that the minimum sulfur content in the gasoline hydrotreating product of 0.0005% was achieved on the catalyst CoO-WO3-La-P-HZSM-HY-Al2O3, which is significantly lower than for other studied catalytic systems. The obtained results of the sulfur content in the hydrotreating products fully comply with the Euro-5 standard. Thus, the efficiency of hydrotreating the gasoline fractions studied in this work was mainly determined by the nature of the carriers and modifiers used for the synthesis of catalysts and the technological parameters of the process. The synthesized catalysts showed high activity and selectivity, resulting in high-octane gasoline with a low sulfur content that meets international quality standards.