Tropical forests are global biodiversity hotspots and are crucial in the global carbon (C) cycle. Understanding the drivers of aboveground carbon stock (AGC) in a heterogeneous and biodiverse system can shed light on the processes underlying the relationship between biodiversity and carbon accumulation. Here, we investigate how biodiversity, environment, and landscape structure affect AGC. We examined such associations in 349 plots comprising over 95,346 km2 the Atlantic Forest of southern Brazil, encompassing three forest types: Dense Ombrophylous Forest (DF), Mixed Ombrophylous Forest (MF), and Seasonal Deciduous Forest (SF). Each plot was described by environmental variables, landscape metrics, and biodiversity (species richness and functional diversity). We used diversity, environmental, and landscape variables to build generalized linear mixed models and understand which can affect the forest AGC. We found that species richness is associated positively with AGC in all forest types, combined and separately. Seasonal temperature and isothermality affect AGC in all forest types; additionally, stocks are positively influenced by annual precipitation in SF and isothermality in MF. Among landscape metrics, total fragment edge negatively affects carbon stocks in MF. Our results show the importance of species diversity for carbon stocks in subtropical forests. The climate effect was also relevant, showing the importance of these factors, especially in a world where climate change tends to affect forest stock capacity negatively.