ABSTRACT. We carry out a systematic theoretical investigation of Magneto Crystalline Anisotropy (MCA) of L1 0 FePt clusters with alternating Fe and Pt planes along the (001) direction. The clusters studied contain 30 -484 atoms. We calculate the structural relaxation and magnetic moment of each cluster by using ab initio spin-polarized density functional theory (DFT), and the MCA with both the self-consistent direct method and the torque method. We find the two methods give equivalent results for all the structures examined. We find that bipyramidal clusters whose central layer is Pt have higher MCA than their same-sized counterparts whose central layer is Fe. This results from the fact that the Pt atoms in such configurations are coordinated with more Fe atoms than in the latter. By thus participating in more instances of hybridization, they contribute higher orbital moments to the overall MCA of the unit. Our findings suggest that by properly tailoring the structure, one can avoid encapsulating the FePt L1 0 nanoparticles, as has been proposed earlier to protect a high and stable magnetic anisotropy. Additionally, using a simple model to capture the thermal behavior, we predict that a five-layered nanoparticle with approximately 700 atoms can be expected to be useful in magnetic recording applications at room temperature.