In this study, Co nanoparticles were deposited on a substrate in an island pattern using an arc plasma gun (APG). An MgO thin film was then formed on this substrate by metal organic decomposition (MOD), which enables the formation of films in atmosphere, thus yielding a double-layer structure. The MgO thin film on Co nanoparticles deposited using an APG with 500 pulses of arc discharge exhibited improved crystallinity and a photoelectron emission that was at least threefold higher than that of the MgO thin film without Co nanoparticles. It was confirmed that depositing Co nanopaticles and then forming the films on them significantly improves characteristics of the MgO thin films. We successfully established a bottom-up process that requires no ion injection by dispersing Co nanoparticles within the MgO thin film during heat treatment.