The need for nontoxic, cheap, earth-abundant catalysts, which can be sustainably produced and implemented, is essential to many processes. In this work we present unsupported iron nanoparticles as an efficient catalyst for selective acetylene hydrogenation under industrially relevant front-end conditions. Additionally, the selectivity and the activity of this catalyst can be easily moderated by the addition of carbon monoxide. The iron nanoparticles were prepared in an environment completely free of water or air using condensed ammonia at −78 °C. State of the art X-ray diffraction and scanning electron microscopy were used to determine the crystal structure, morphology, and purity. The catalyst showed stable performance over several experiments and, other than an agglomeration of the unsupported and unstabilized particles, no changes to the catalyst were detected before and after the reactions.