The conversion of the straight-run gasoline fraction of high-paraffin crude oil into the high-octane gasoline over niobium-zirconium-aluminosilicate catalyst with the ZSM-5 zeolite structure has been studied. The influence of the process conditions on the yield, composition, and performance characteristics of the product gasoline has been shown. It has been found that in the presence of the catalyst, the required quality of gasoline can be reached by varying the process conditions. Using ammonia thermal desorption and differential thermal analysis techniques, data on the acid characteristics of the zeolite catalyst and the amount of coke formed on its surface during the conversion of straight-run gasoline have been obtained. The catalyst operation stability in the model reaction of methanol-to-hydrocarbons conversion has been estimated.