Based on much experimental and theoretical work in the last decade or so, mechanical properties of materials at nano-scale are proving to significantly deviate from their bulk counterparts. This is true not only for nano-structureD materials (i.e. composed of nano-scale components like nanocrystalline materials) but also for nano structureS (surface-dominated structures like carbon nanotubes (CNT’s), nanowires, etc.). Nanoindentation has been a very effective and well-characterized technique for determination of hardness, modulus, and stiffness, and for crystalline materials the indentation hardness has been widely shown to be significantly higher at shallower indentation depths (so-called indentation size effect, or ISE). However, inserting a sharp indenter tip into a material inevitably sets up strong strain gradients in the deforming volume, which is often linked to the origin of the ISE. Moreover, the infinitesimal volumes probed via this technique are coherent with the remaining matrix, rendering the effects of free surfaces on mechanical properties inaccessible.