The effect of seed layers on the magnetic and structural properties of FePt thin films was investigated. For the case of Cr(200) seed layer, no ordered L10‐FePt phase in (001) orientation was observed. The insertion of a thin MgO barrier between the Cr and FePt layers improved the perpendicular magnetization orientation of L10‐FePt by limiting diffusion of Cr into the FePt magnetic layer. Ordered L10‐FePt thin films can be developed on Pd[100] at high substrate temperature with the lattice mismatch of below 1% and therefore low roughness compared to MgO or Cr seed layers. (© 2011 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)