The Fe-coating and H-2-annealed processes markedly increased the conductivity and enhanced the surface electron field emission (s-EFE) properties for the diamond films. The enhancement on the s-EFE properties for the diamond films is presumably owing to the formation of nano-graphite clusters on the surface of the films via the Fe-to-diamond interaction. However, the extent of enhancement varied with the granular structure of the diamond films. For the microcrystalline (MCD) films, the s-EFE process can be turned on at (E-0)(MCD) = 1.9 V/mu m, achieving a large s-EFE current density of (J(e))(MCD) = 315 mu A/cm(2) at an applied field of 8.8 V/mu m. These s-EFE properties are markedly better than those for Fe-coated/annealed ultrananocrystalline diamond (UNCD) films with (E-0)(UNCD) = 2.0 V/mu m and (J(e))(UNCD) = 120 mu A/cm(2). The transmission electron microscopy showed that the nano-graphite clusters formed an interconnected network for MCD films that facilitated the electron transport more markedly, as compared with the isolated nano-graphitic clusters formed at the surface of the UNCD films. Therefore, the Fe-coating/annealing processes improved the s-EFE properties for the MCD films more markedly than that for the UNCD films. The understanding on the distribution of the nano-clusters is of critical importance in elucidating the authentic factor that influences the s-EFE properties of the diamond films. Such an understanding is possible only through the 3D-tomographic investigations. Copyright 2012 Author(s). This article is distributed under a Creative Commons Attribution 3.0 Unported License. [http://dx.doi.org/10.1063/1.4748865]