In recent years, nanomaterials have shown great potential in the enhanced oil recovery (EOR) process due to their superior properties. However, the influence of particle size on EOR is not clear and hinders the application. Therefore, it is vitally important to investigate the effect of the particle size on the EOR performance. In this work, Fe3O4 nanoparticles with different sizes, including 20 nm, 100 nm, 200 nm, and 300 nm, were controllably synthesized and used to innovatively clarify the critical role of nanoparticles size in enhancing oil recovery. The effects of sizes on the recovery were investigated by combining the experimental results of interfacial tension, wetting angle, and spontaneous imbibition. The results revealed that Fe3O4 nanoparticles with smaller size, which have the stronger ability to reduce the interfacial tension and change the wetting angle, exhibit a favorable capacity to enhance oil recovery. Compared with the spontaneous imbibition oil recovery (24.36 %) of standard brine, the nanofluid containing 0.1 wt% Fe3O4 with the size of 20 nm can increase the recovery to 30.87 %. Based on the results of nuclear magnetic resonance, the spontaneous imbibition mechanism was proposed and the effect of size on recovery was analyzed. In addition, the superparamagnetism of Fe3O4 was utilized for recycling, avoiding the issue of significant losses of nanofluids in the existing research after injection. The secondary spontaneous imbibition was carried out, showing good environmental friendliness.