A series of paramagnetic di(aryl)alkynylphosphine oxides 3a–c[PF₆] featuring an open-shell [Fe(κ²-dppe)(η⁵-C₅Me₅)]⁺ endgroup were obtained by oxidation of their neutral Fe(II) parents 3a–c, themselves obtained in a simple and nearly quantitative fashion from the corresponding Fe(II) metallophosphines 1a–c. The new organometallic radicals were characterised by NMR and ESR and were shown to be perfectly stable in solution, in contrast to species such as 1a–b[PF₆] which readily dimerise.