In order to improve the interlaminar mechanical properties of CFRP laminate, hybrid CFRP/VGCF laminates have been fabricated by newly-developed powder method. The critical load at crack growth Pc and fracture toughness GIC have been found to be increased with VGCF interlayer through double cantilever beam (DCB) tests. Fracture surfaces of DCB specimens have also been observed to interpret this improvement mechanism. Moreover, numerical simulations using finite element method (FEM) with cohesive elements have been carried out to analyze the delamination propagation. The numerically obtained interlaminar tensile strength of hybrid CFRP/VGCF laminates has also been verified to be higher than that of base CFRP laminates.