Research on the synergistic high-value reuse of waste tires and used catalysts in spent fluid catalytic cracking (FCC) catalysts was carried out in this study to address the serious ecological and environmental problems caused by waste tires and spent FCC catalysts. The experiment, in which a spent FCC catalyst was applied to the catalytic cracking of waste tires, fully utilized the residual activity of the spent FCC catalyst and was compared with a waste tire pyrolysis experiment. The comparative experimental results indicated that the spent FCC catalyst could improve the cracking efficiency of waste tires, increase the output of light oil in pyrolysis products, and improve the quality of pyrolysis oil. It could also be used for the conversion of sulfur compounds during cracking. The content of 2-methyl-1-propylene in catalytic cracking gas was found to be up to 65.59%, so a new method for producing high-value chemical raw materials by the catalytic cracking of waste tires with spent FCC catalysts is proposed.