We report tight-binding and density functional theory calculations of magnetocrystalline anisotropy energy (MAE) of free Fe (body-centered-cubic) and Co (face-centered-cubic) slabs and nanocrystals. The nanocrystals are truncated square pyramids which can be grown experimentally by deposition of metal on a SrTiO3(001) substrate. For both elements our local analysis shows that the totalMAE of the nanocrystals is largely dominated by the contribution of (001) facets. However, while the easy axis of Fe(001) is out-of-plane, it is in-plane for Co(001). This has direct consequences on the magnetic reversal mechanism of the nanocrystals. Indeed, the very high uniaxial anisotropy of Fe nanocrystals makes them a much better potential candidate for magnetic storage devices.