The Huangjindong gold deposit in northeastern Hunan is one of the most representative gold deposits in the Jiangnan Orogenic Belt. The orebodies are mainly hosted in the Neoproterozoic Lengjiaxi Group, which comprises carbonaceous slates. Abundant carbonaceous material (CM) can be found in the host rocks and ore-bearing quartz veins, but its geological characteristics and genesis, as well as its association with gold mineralization, are still unclear. Systematic petrographic observation demonstrated two types of CM in host rocks and ores, i.e., CM1 and CM2. Among them, CM1 is the predominant type and mainly occurs in the layered carbonaceous slates, while CM2 is mostly present in quartz veins and mineralized host rocks. Laser Raman spectroscopic analyses of CM1 were performed at higher temperatures (376–504 °C), and CM2 was generated at similar temperatures (255–435 °C) to gold mineralization. Combined with previous studies, we can conclude that CM1 was produced by Neoproterozoic to early Paleozoic metamorphism before gold mineralization, while CM2 is of hydrothermal origin. Geochemical modeling indicates that CM1 could promote gold precipitation through reduction, as well as facilitate structure deformation and metal absorption as previously proposed. However, hydrothermal CM2 is favorable for gold mineralization because it triggers sulfidation, similar to other Fe-bearing minerals (such as siderite) in the host rocks. Consequently, both types of CM in the Huangjindong deposit are favorable for gold mineralization and carbonaceous slates could be important gold-bearing units for future ore prospecting in the Jiangnan Orogen as well as other places in South China.