The measurement of bolt preload by using ultrasound can be accurate, convenient, and can realize the real-time monitoring of the change in the residual axial stress of a bolt during use. In order to realize the ultrasonic measurement of bolt preload, the use of zinc oxide (ZnO) piezoelectric thin-film material as an ultrasonic transducer material to stimulate an ultrasonic signal on the bolt is a feasible solution. In this paper, we choose to use RF magnetron sputtering technology to prepare ZnO piezoelectric thin-film materials and study the effects of sputtering power and target substrate distance on the structure and ultrasonic properties of ZnO piezoelectric thin films during the preparation process, in order to lay the foundation for realizing the application of ZnO piezoelectric thin films in the field of bolt preload measurement. The experimental results show that too-large sputtering power or too-small target substrate distance will result in the particles having too much kinetic energy during sputtering and exhibiting a structure of multiorientation growth, which excites ultrasonic longitudinal–transverse waves. A sputtering power of 600 W, sputtering time of 4 h, and target substrate distance of 100 mm are ideal experimental parameters for a ZnO piezoelectric thin-film material to be excited by an ultrasonic longitudinal wave signal, and its ideal operating frequency is 41 MHZ. These research results of bolt stress detection demonstrate good application prospects.