In the presence of graphene oxide (GO), highly crystallized SAPO-11 molecular sieves were prepared by a non-solvent method. The functional groups of GO bind with raw materials, with the formation of hydrogen bonds and acid amides, verified by the XPS analysis. The inorganic precursor and structure-directing agent molecules will be fixed on the surface of GO, increasing the reaction rate and crystallization for SAPO-11 preparation, confirmed by the XRD and BET results. Meanwhile, the IR analysis of the adsorption of pyridine indicates there are more acidic sites for the highly crystallized SAPO-11 sample. The resultant well-crystallized SAPO-11 molecular sieves exhibited greater isomer yield and better catalytic activity compared to traditional SAPO-11 prepared without GO.