An experimental investigation of the effects of pre-bond contamination on Mode-I fracture toughness of carbon fiber reinforced plastic (CFRP) bonded joints is presented in this paper. Two pre-bond contamination scenarios were considered; namely, the silicon-based release agent and moisture. The two contamination scenarios were realized in one of the composite substrates prior to bonding. The common characteristic of the two contamination scenarios is that they lead in the formation of defects in the form of weak bonds that cannot be detected by conventional non-destructive testing techniques. The contamination effects on Mode-I fracture toughness of the bonded joints were investigated by conducting mechanical tests on double-cantilever beam specimens and comparing the results with relative measurements taken from reference specimens. Prior to mechanical testing, the bonding quality of the specimens was tested using ultrasonic C-scan inspection. Both the release agent and moisture are found to significantly degrade the Mode-I fracture toughness of the joints. For the release agent, the effect was more significant for silicon concentrations over 5 at%; a complete lack of adhesion was observed for silicon concentrations over 7 at%. At low values of relative humidity, there was a small increase in Mode-I critical energy release rate while at larger values there is a decrease which reaches 26% for the higher relative humidity percentage. The results from the Non-Destructive Testing (NDT) tests verify the inability of conventional NDT to detect the defects resulting at the interface between the contaminated adherend's surface and the adhesive for both contamination scenarios.