Iron bis(N,N'-diisopropylacetamidinate) [Fe-2(mu-Pr-i-MeAMD)(2)(eta(2)-Pr-i-MeAMD)](2) and iron bis (N,N'-di-tert-butylacetamidinate) [Fe(Bu-t-MeAMD)(2)] were used as precursors for the metallorganic chemical vapor deposition (MOCVD) of iron-containing compounds including pure iron, iron carbides, Fe3C and Fe4C, and iron nitrides Fe4C. Their decomposition mechanism involves hydrogen migration followed by dissociation of the Fe-N bond and the release of free hydrogenated ligand (HL) and radicals. Surface intermediates are either released or decomposed on the surface providing Fe-N or Fe-C bonds. MOCVD experiments were run at 10 Torr, in the temperature ranges of 350-450 degrees C with Fe-2(mu-Pr-i-MeAMD)(2)(eta(2)-Pr-i-MeAMD)(2) and 280-350 degrees C with Fe(Bu-t-MeAMD)(2). Films prepared from Fe-2(mu -Pr-i-MeAMD)(2)(eta(2)-Pr-i-MeAMD)(2) contain Fe, Fe3C, and Fe4C. Those prepared from Fe(Bu-t-MeAMD)(2) contain Fe, Fe3C, and also Fe4C or Fe4N, depending on the temperature and hydrogen to precursor ratio (H/P) in the input gas. The room-temperature coercive field of films processed from Fe(Bu-t-MeAMD)(2) is 3 times higher than that of the high temperature processed Fe4N films. (C) 2010 The Electrochemical Society. [DOI:10.1149/1.3430105] All rights reserved.