Hard and brittle material components with complex curved surfaces are widely used in critical foundational parts within aerospace, optoelectronics, and other fields. Their machining quality directly determines the performance and reliability of high-end equipment. However, the inherent properties of hard and brittle materials make them prone to surface/subsurface damage during traditional polishing processes, and maintaining the form accuracy of complex curved surfaces is challenging. Although abrasive waterjet polishing enables non-contact flexible processing, its energy efficiency is low. Additionally, although ultrasonic-assisted polishing can improve material removal, its spatial localization is insufficient, limiting energy utilization efficiency. To address these issues, this paper proposes a novel method of focused, ultrasonic, vibration-assisted abrasive waterjet polishing. The influence of the radiation force and cavitation force of the focused ultrasonic field on abrasive particle motion is analyzed, and analytical equations for abrasive particle velocity are established. Subsequently, single-factor and response surface methodologies are employed to systematically evaluate the influence of process parameters on machining quality and efficiency. The material removal process during FUAP involves both plastic shearing/chip formation and localized brittle fracture. Focused ultrasonic assistance promotes micro-cutting and plastic shearing, while localized crushing pits indicate that brittle fracture remains non-negligible. The focused ultrasound superimposes alternating stress onto the impact action, mitigating microscale crushing pit defects during the brittle removal process of monocrystalline silicon. Furthermore, appropriately increasing ultrasonic power, enlarging abrasive particle size, and raising abrasive concentration all contribute to enhanced material removal from monocrystalline silicon. Adjusting the nozzle height to the effective region of the focused ultrasonic energy field promotes material removal via chip formation while avoiding pit defects caused by excessive fracture. These results suggest that focused ultrasonic energy can be effectively integrated into abrasive waterjet polishing to enhance material removal while suppressing brittle surface defects, thereby offering a promising strategy for the ultra-precision finishing of hard and brittle components with complex curved surfaces.