Vibration monitoring is one of crucial functions of structural health monitoring (SHM) systems. Traditional structural vibration monitoring usually relies on specialized sensors, data transmission and acquisition equipment, which are expensive and may not be easily available in urgently needed situations like post-disaster structural evaluation. Therefore, developing an affordable and efficient structural vibration monitoring technique becomes an important topic in SHM research. In this paper, the authors developed an android system APP that can easily convert multiple android smartphones into a wireless structural vibration monitoring system. To make the designed system reliable and easy to use, the server/client architecture is adopted. One smartphone is designated as the serve of the system to remotely control all other smartphones, which function as sensors to measure structural vibration. An efficient method is proposed herein to establish the smartphone-based structural vibration monitoring network, allowing the server smartphone to quickly and easily connect multiple sensor smartphones to form the wireless network for structural vibration monitoring. Additionally, a synchronization method is also proposed to synchronize different smartphones for simultaneously measuring structural vibration. To verify the time synchronization accuracy of the developed system, an experiment is designed and conducted. Moreover, a new analysis method of the time synchronization accuracy is also proposed, which verifies that the designed smartphone-based monitoring can achieve the millisecond-level time synchronization accuracy. Finally, a shaking table experiment is conducted on a three-story bench-scale structural model, the results of which demonstrate that the designed smartphone-based wireless structural vibration monitoring system can quite accurately identify the modal parameters of the tested structure.