To achieve ultrasonic transducers operating above 100 MHz, square pillar shaped Pb1.1(Zr0.53Ti0.47)O3 thick film structures were fabricated using a chemical solution deposition (CSD) process. The fabricated sample showed well-saturated P-E hysteresis curve and butterfly-shaped longitudinal displacement curve. The fabricated samples generated more than 100 MHz ultrasonic waves with a pulser/receiver. Electrical impedance properties of the samples were measured with an impedance analyzer. A number of spurious resonant modes were observed in the frequency range from 40 to 300 MHz. The characteristics of the sample were investigated by finite element method (FEM). The FEM simulations were in good agreement with the experimental results. For free-standing (substrate free) 10-μm-thick PZT film models, the resonant frequency of the thickness vibration mode was estimated to be 160 MHz with the FEM simulations. These results indicate that the substrate affects the behavior of the spurious resonant modes. Therefore, a sample structure was designed using the FEM simulation. The FEM result suggests that the backside of the substrate should be removed to reduce the substrate effects. Consequently, the thickness vibration mode was observed clearly at 160 MHz. This structure is applicable to the micromachined ultrasonic transducers (MUT) operating in the thickness vibration mode above 100 MHz.