In order to improve the interlaminar mechanical properties of CFRP laminates, hybrid CFRP/VGCF laminates have been fabricated by using a newly-developed method, i.e., powder method, where the powder of vapor grown carbon fiber (VGCF) is added at the mid-plane of [0°/0°] 14 CFRP laminates. Experimental results of double cantilever beam (DCB) tests indicate the improvement on the interlaminar mechanical properties of Mode-I fracture behavior with much higher critical load P C and fracture toughness G IC with VGCF interlayer. Crack propagation and fracture surface have also been observed to interpret this improvement mechanism. Moreover, based on experimental G IC , numerical simulations using finite element method (FEM) with cohesive elements have been carried out to analyze the delamination propagation. The interlaminar tensile strength of hybrid CFRP/VGCF laminates, which is obtained by matching the numerical load–COD (crack opening displacement) curves to experimental ones, is higher than that of base CFRP laminates.