Cavitation will cause abnormal flow, causing a series of problems such as vibration, noise, and erosion of solid surfaces. In severe cases, it may even destroy the entire system. Cavitation is a key problem to be solved for hydraulic machinery and underwater robots, and the attack angle is one of the most important factors affecting the cavitation. In order to systematically study the impact of the attack angle on the hydrofoil cavitation, the hydrofoils of NACA 4412 with different attack angles were selected to study the collapse process and hydraulic characteristics such as pressure, velocity, vortex, and turbulent kinetic energy during cavitation. The results showed that when the cavitation number was the same, the process of cavity collapse was greatly affected by the attack angle. The length of the cavity collapse area was positively correlated with the attack angle. As the attack angle increased, the volume of the falling bubbles increased, resulting in a larger pressure peak caused by the collapse of bubbles. Moreover, the pressure gradient near the collapse point changed more drastically, thereby affecting the growth of attached cavitation. The fluctuation range of vortex core and turbulent kinetic energy also increased with increasing the attack angle.