This research aimed to investigate the effects of an ultrasonic surface rolling process (USRP) on the deposition behaviors in CaCO3 crystallization fouling for 304 stainless steel (304SS). The microstructure, surface morphology, and hydrophobic properties of the modified layer were characterized with optical microscopy, a roughness profile measurement instrument, and a contact angle measurement instrument. The corrosion and fouling behaviors of different surfaces were studied in simulated cooling water. The polarization curves and electrochemical impedance spectroscopy (EIS) were used to evaluate the electrochemical properties. The results showed that USRP-treated surfaces had better anti-corrosion and anti-fouling performance. The improvement in anti-fouling performance was attributed to the weakening of peaks and valleys, the reduction of surface defects, and the improvement of corrosion resistance.