Many operations in power grids, such as fault detection and event location estimation, depend on precise timing information. In this paper, a novel Time Synchronization Attack (TSA) is proposed to attack the timing information in smart grid. Since many applications in smart grid utilize synchronous measurements and most of the measurement devices are equipped with global positioning system (GPS) for precise timing, it is highly probable to attack the measurement system by spoofing the GPS. The effectiveness of TSA is demonstrated for three applications of phasor measurement unit (PMU) in smart grid, namely transmission line fault detection, voltage stability monitoring and event locationing. The validity of TSA is demonstrated by numerical simulations.