The aim of this study was to investigate the bond strength between thermoplastic carbon fiber reinforced polymers (CFRP) and aluminium alloys with different surface modifications. The materials examined were unidirectional carbon fiber reinforced polyamide-6 composites and two different types of aluminium alloys. The configuration chosen for studying the interfacial adhesion is symmetrical with one 0.3 mm thick aluminium foil at the neutral axis of the stack. Various surface modifications like laser structuring, diamond-like carbon (DLC) coating, corundum blasting and different chemical treatments were performed on the aluminium layer. In addition, polyamide-6 interlayers with and without glass-fibres were investigated as an electrochemically insulating layer between aluminium and carbon fibres. The specimens were evaluated using a short beam 3-point bending test to determine the apparent interlaminar shear strength (ILSS). For this purpose, three groups of specimens were stored under standard climate, in a vacuum oven and in hot/wet conditioning for one week, respectively In addition, potentiodynamic corrosion measurements were performed on the aluminium alloys to evaluate the electrochemical barrier resulting from surface treatments and interlayers. It was observed that 1050 aluminium alloys performed better than 2014 alloys in this aspect. Interlayers with glass fibres had slightly lower ILSS values with mainly cohesive interfacial failure.