In order to understand the mechanical behaviour of Al2O3 inverse opals, nanoindentation techniques have been implemented in material layers with three different microstructures, in terms of hollow or polystyrene spheres, with Al2O3 shells of distinct wall thickness. Different indenter tip geometries as well as contact loading conditions have been used, in order to induce different stress field and fracture events to the layers. Field emission scanning electron microscopy and focused ion beam have been employed to understand accommodation of plastic deformation induced during the indentation process. Results show that materials with polystyrene spheres exhibit higher hardness and modulus under sharp indentation, and cracking resistance under spherical indentation. Furthermore, deformation is discerned to be mainly governed by the rotation of the microspheres. In the case of the inverse opals made of hollow spheres, the main deformation mechanisms activated under indentation are the rearrangement and densification of them