In view of the severe coke formation and catalyst deactivation during crude bio-oil cracking, an innovative cracking technology based on bio-oil molecular distillation is proposed. The distilled fraction (DF) from bio-oil molecular distillation is enriched with small molecular acids and ketones and has enhanced cracking behavior compared to crude bio-oil. The influence of the reaction temperature, pressure, and the DF/ethanol ratio in the feed was studied. It was found that co-cracking of the DF and ethanol produced a well-defined gasoline phase, and both increasing the reaction temperature and adopting pressurized cracking benefited the yield and quality of this gasoline phase. Using optimum reaction temperature and pressure, co-cracking of the DF and ethanol, with different weight ratios, all generated high-quality gasoline phases. Under 400 degrees C and 2 MPa, co-cracking of DF and ethanol with a weight ratio of 2:3 produced a high gasoline phase yield of 25.9 wt %; the hydrocarbon content in this gasoline phase was 98.3%.