Due to advantages such as light weight, flexibility, and low cost, polyvinylidene fluoride (PVDF) films have been widely used in engineering applications as sensors for detecting strain, pressure, or micro-force. However, it is known that PVDF strain sensors have strain cross-sensitivity in mutually orthogonal directions. Furthermore, the size of the PVDF film sensor would also affect the dynamic strain sensing performance. In this paper, to investigate the cross-sensitivity and size effects experimentally, we employ PVDF film sensors to perform dynamic measurements on a cantilever beam. Since the vibrations of the cantilever beam are excited by impacts of a steel ball, the induced highly repeatable transient responses contain a wide range of resonant frequencies and thus can be used to investigate both the size and cross-sensitivity effects of the PVDF film sensors in a dynamic sensing environment. Based on the experimental results of the identified resonant frequencies compared with results obtained from a strain gauge, finite element calculations, and theoretical predictions, suggestions for the use of the PVDF strain sensor in modal testing are given in this paper.