The carbon nanotube (CNT) and graphene oxide are widely applied in Glass Fiber Reinforced Polymer (GFRP) to enhance interlaminar performance, even though they have an extremely expensive price. Herein, we provide a novel interlaminar toughening material: carbon black, which has a cheap price and good interlaminar properties. The relationship between different amounts of three nanomaterials and toughening efficiency is obtained through experiments (end notch bending (ENF) test) and the curves between different amounts and prices are revealed by the investigation. Moreover, a mathematical model of interlaminar performance, material consumption, and price is established, which can provide researchers with accurate, efficient, and inexpensive predictions in different application environments. On the other hand, a simple and efficient spraying method for making reinforcement layers is adopted in this research and we analyzed the microstructure strengthening mechanism of three nanomaterials by scanning electron microscopy (SEM).