Nanoindentation has been used to characterize the mechanical properties of aerospace-grade Al2024-T351 with and without a clad layer of pure aluminium. The clad layer is introduced by means of a roll-bonding process which can cause significant work-hardening of the material in the clad layer. The hardness and Young's modulus of the pure aluminium and the Al2024 have been determined by a number of methods, including the traditional Oliver and Pharr method, and a number of other methods, including direct measurement of the indentation by atomic force microscopy, and evaluation of the work of indentation. The Oliver and Pharr method was found to underestimate the area of contact as it did not include the area of piled-up material around the indentation periphery. This gave a corresponding overestimation of both hardness and modulus. The area of the indentation measured by atomic force microscopy was similarly found to underestimate the contact area owing to relaxation of material around the indent between indentation and imaging. The work of indentation approach was found to give good agreement between the hardness calculated by nanoindentation and those found in the literature.