Competitive hydrogenation of mixtures of unsaturated compounds is a topical area of research, mainly due to their continued presence in industrial feedstocks. Here, we investigate the effects of coating a catalyst with the ionic liquid 1,3-dimethylimidazole methyl sulfate [MMIM][MeOSO3] at various isoconversions in the competitive hydrogenation of 1-octyne versus 1-octene. Our results indicate that solid catalyst with an ionic liquid layer (SCILL) catalysts offer advantages compared to the uncoated versions. We also investigated some of the difficulties in creating SCILL catalysts which can lead to catalyst deactivation, with crystallite morphologies appearing to play a role in catalyst deactivation with time on exposure to the atmosphere.