The effect of a chemical pretreatment on the surface carbon was investigated using a scanning electron microscope (SEM) and electrochemical methods. Primitive carbon has a reducing power likely due to incompletely oxidized functional groups on the surface. We aim to control this reducing power by chemical treatment and apply for the spontaneous deposition of nanoparticles (NPs). Highly ordered pyrolytic graphite (HOPG) was initially treated with a reducing agent, NaBH4 or an oxidizing agent, KMnO4, for 5 min. Subsequently, the pretreated carbon was immersed in a platinum (Pt) precursor. Unexpectedly, SEM images showed that the reducing agent increased spontaneous PtNPs deposition while the oxidizing agent decreased Pt loading more as compared to that of using bare carbon. However, the amount of Pt on the carbon obviously decreased by NaBH4 treatment for 50 min. Secondly, spontaneous reduction on pretreated glassy carbon (GC) was investigated using the catalytic hydrogen evolution reaction (HER). GC electrode treated with NaBH4 for a short and long time showed small (onset potential: -640 mV vs. MSE) and large overpotential for the HER, respectively. Although the mechanism is unclear, the electrochemistry results correspond to the optical data. As a proof-of-concept, these results demonstrate that chemical treatments can be used to design the shapes and amounts of deposited catalytic metal on carbon by controlling the surface state.