One of the major challenges in manufacturing automotive lithium-ion batteries and battery packs is to achieve consistent weld quality in joining multiple layers of dissimilar materials. While most fusion welding processes face difficulties in such joining, ultrasonic welding stands out as the ideal method. However, inconsistency of weld quality still exists because of limited knowledge on the weld formation through the multiple interfaces. This study aims to establish real-time phenomenological observation on the multilayer ultrasonic welding process by analyzing the vibration behavior of metal layers. Such behavior is characterized by a direct measurement of the lateral displacement of each metal layer using high-speed images. Two different weld tools are used in order to investigate the effect of tool geometry on the weld formation mechanism and the overall joint quality. A series of microscopies and bond density measurements is carried out to validate the observations and hypotheses of those phenomena in multilayer ultrasonic welding. The results of this study enhance the understanding of the ultrasonic welding process of multiple metal sheets and provide insights for optimum tool design to improve the quality of multilayer joints.