The use of light composites when designing fast moving parts for machine tools is emerging as a very efficient solution for improving productivity. Nevertheless, several aspects of these materials have to be carefully considered in woodworking. This paper aims to investigate the effect of interleaved nanofiber on mode I interlaminar properties and the failure modes that occur in this mode. For this purpose, woven carbon/epoxy laminates with and without Polyvinylidene difluoride nanofibers in the mid-plane were subjected to mode I interlaminar loading and the results were compared with each other. Acoustic emission technique was also utilized for better understanding of the failure modes that occurred in the virgin and nanofibers-modified specimens. Mechanical data and acoustic emission parameters associated with pattern recognition analyses were used for investigation of the interlaminar properties and the occurred failure modes. The mechanical results showed that the electrospun nanofibrous mat was able to increase the GIC by 98%. The acoustic emission results highlighted that different failure modes were the origin of different interlaminar failure behaviors. Different percentages of the failure modes in the modified specimens compared with the virgin ones were observed. Furthermore, the number of occurred interlaminar failure modes diminished in the modified composite layers.