In this work, the impact behavior of the electrified carbon fiber reinforced polymer (CFRP) composites with carbon nanotube (CNT) buckypaper layers has been studied. A custom-built experimental setup that allows for real time measurements of pulsed electric current, voltage, load, and velocity during coordinated application of a current pulse with an impact load was utilized. The experimental setup included a current pulse generator capable of producing a 30 millisecond current pulse with an amplitude of up to 2500 A. The application of the peak of the current pulse was coordinated with the peak of the impact load. A series of electrical, impact, and coordinated electrical-impact characterization tests were performed on three types of samples: 16-ply IM7/977-3 unidirectional laminates; laminates containing four layers of buckypaper (BP) and 12 unidirectional IM7/977-3 layers arranged as CF2/BP/CF4/BP/CF4/BP/CF4/BP/CF2; and laminates containing seven layers of buckypaper and nine unidirectional IM7/977-3 layers arranged as [CF2/BP]7/CF2. The results show that addition of buckypapers can lead to the increased impact resistance of CFRP composites.