Understanding the drivers of variations in carbon stocks is essential for developing the effective management strategies that contribute to mitigating climate change. Although a positive relationship between biodiversity and the aboveground carbon (AGC) has been widely reported for various Brazilian forest types, representing a win-win scenario for climate change mitigation, this association has not been commonly found in Brazilian subtropical forests. Therefore, in the present study, we aimed to evaluate the effects of Araucaria angustifolia, stand structure and species diversity in shaping AGC stocks in Brazilian subtropical mixed forest. We hypothesized that the effects on the AGC of stand structure and diversity would be mediated by A. angustifolia. We also evaluated the expectation of higher carbon stocks in protected forest as a result of their positive correlation with biodiversity conservation. We found that stand structure, followed by A. angustifolia, played the most important role in shaping the AGC stock. Our hypothesis was partially confirmed, the indirect effects of A. angustifolia on stand structure being found to have shaped the AGC. Similarly, our expectation was partially supported, with the higher AGC in the protected area being related not to diversity, but rather to the presence of larger trees, denser stands, and a greater abundance of A. angustifolia. Although the win-win strategy between diversity conservation and carbon storage is not a peculiarity of Araucaria forests, we highlight the potential of these forests as a nature-based climate solution, maintaining high levels of carbon storage in harmony with the provision of keystone socio-economic resources.