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"Interleaving" is widely used for interlaminar toughening of fiber-reinforced composites, and the structure of interleaving is one of the important factors affecting the toughening efficiency of laminates. Several experiments have demonstrated that compared to continuous and dense structures, toughening layers with structural heterogeneity can trigger multiple toughening mechanisms and have better toughening effects. On this basis, this work further investigates the application of heterogeneous toughening phases in interlaminar toughening of bidirectional GFRP. CNT was selected to construct toughening phases, which was introduced into the interlaminar of composites through efficient spraying methods. By controlling the amount of CNT, various structures of CNT toughening layers were obtained. The fracture toughness of modified laminates was tested, and their toughening mechanism was analyzed based on fracture surface observation. The results indicate that the optimal CNT usage (0.5 gsm) can increase the initial and extended values of interlayer fracture toughness by 136.0% and 82.0%, respectively. The solvent acetone sprayed with CNT can dissolve and re-precipitate a portion of the sizing agent on the surface of the fibers, which improves the bonding of the fibers to the resin. More importantly, larger discrete particles are formed between the layers, guiding the cracks to deflect in the orientation of the toughened layer. This generates additional energy dissipation and ultimately presents an optimal toughening effect. [ABSTRACT FROM AUTHOR]