Aiming to increase damage tolerance of adhesively bonded joints, this work explores the influence of CFRP layup of the adherends on the crack onset and crack propagation of composite bonded joints under mode I loading. Quasi-static Double Cantilever Beam tests were performed using four different CFRP layups bonded with two adhesives. Parallel to the experimental program, finite element analyses were performed to aid in understanding and identifying the various damage mechanisms in each specimen type. The results show that the CFRP layup and adhesive fracture toughness significantly influence the joint fracture phenomena at crack onset and further crack propagation. An enhancement of the joint's mode I fracture toughness values at crack onset was observed in the specimens where a crack competition between the propagation within the bondline and the composite's layers was triggered. During crack propagation, the fracture toughness of the joint increases at crack deflections between the different plies of the CFRP layup until reaching the 0° ply, where sudden delamination occurs. It has been shown that CFRP layup tailoring is a promising toughening method that, when carefully designed, has the potential to increase the maximum effective fracture toughness up to 100% when compared to pure cohesive failure.