This paper presents a feasibility study of flexible piezoelectric paint for use in wide-band low-profile surface-mount or embeddable ultrasonic sensor for in situ structural health monitoring. Piezoelectric paint is a piezoelectric composite with 0-3 connectivity. Because of its ease of application, piezoelectric paint can be readily fabricated into sensing element with complex pattern. This study examines the characteristics of piezoelectric paint in acoustic emission signal and ultrasonic guided wave sensing. A series of ultrasonic tests including pitch catch and pencil break tests were performed to validate the ultrasonic wave sensing capability of piezoelectric paint. The results of finite element simulation of ultrasonic wave propagation, and acoustic emission generated by a pencil lead break on an aluminum plate are also presented in this paper along with corresponding experimental data. Based on the preliminary experimental results, the piezoelectric paint appears to offer a promising sensing material for use in real-time monitoring of crack initiation and propagation in both metallic and composite structures.