The pyrolysis of cylinder-forming samples of the diblock copolymer polystyrene-block-poly(ferrocenylethylmethylsilane) (PS-b-PFEMS) in bulk and in thin films has confirmed that these materials are useful for the generation of semi-ordered arrays of C/SiC ceramics containing Fe nanoparticles which are derived from the organometallic domains. In many cases, the ceramic mass yields were predictable and produced ceramics bearing a monomodal distribution of iron nanoparticles due to the nanoscaled structure of the preceramic PFEMS domains. The pyrolysis of thin films stabilized by cross-linking the PS domains with UV light demonstrated high areal yields, improved shape retention, and the presence of cylinder-centered magnetic nanoparticles.