Atomic layer deposition (ALD) of platinum (Pt) has gained significant interest in the recent years due to its capability of depositing various Pt nanostructures for applications in different fields, such as Pt nanoparticles (NPs) for catalytic reactions and energy devices and Pt thin films for microelectronic technology. Among various developed processes, Pt ALD using MeCpPtMe₃as the precursor has been most popularly employed owing to the high reactivity, volatility, and thermal stability of the precursor, which enable controlled deposition of Pt nanostructures in a broad range of temperatures. Typical MeCpPtMe₃-based Pt ALD processes use O₂and H₂as the coreactants. In this study, we explore atomic hydrogen as an alternative and reveal its exceptional reactivity that outperforms H₂and O₂. Specifically, atomic hydrogen enables the deposition of highly dispersed Pt NPs with narrow particle size distributions (i.e., standard deviation <0.3 nm) on various oxide surfaces, including TiO₂, SiO₂, CeO₂and V₂O₅, which is unattainable with H₂under identical experimental conditions. In addition, it facilitates the deposition of Pt NPs with improved size uniformity and accelerates the closure of Pt films compared to ALD processes using O₂as the coreactant. The results demonstrate a significant potential of atomic hydrogen as a highly effective coreactant for ALD of Pt NPs and thin films.