Methylcyclopentadiene dimer and trimer based fuels are synthesized from 5-methyl furfural for the first time with yields as high as 74.4%. They exhibit both high density and high thermal stability that are better than those of widely used fossil based jet fuels such as JP-10 and JP-7, and represent types of high-performance fuels. This work also provides a potential and scale-up feasible route for synthesizing high-performance jet fuels from biomass.