Afforestation and land use changes that sequester carbon from the atmosphere in the form of woody biomass have turned southern China into one of the largest carbon sinks globally, which contributes to mitigating climate change. However, forest growth saturation and available land that can be forested limit the longevity of this carbon sink, and while a plethora of studies have quantified vegetation changes over the last decades, the remaining carbon sink potential of this area is currently unknown. Here, we train a model with multiple predictors characterizing the heterogeneous landscapes of southern China and predict the biomass carbon carrying capacity of the region for 2002–2017. We compare observed and predicted biomass carbon density and find that during about two decades of afforestation, 2.34 PgC have been sequestered between 2002 and 2017, and a total of 5.32 Pg carbon can potentially still be sequestrated. This means that the region has reached 73% of its aboveground biomass carbon carrying capacity in 2017, which is 12% more than in 2002, equal to a decrease of 0.77% per year. We identify potential afforestation areas that can still sequester 2.39 PgC, while old and new forests have reached 87% of their potential with 1.85 PgC remaining. Our work locates areas where vegetation has not yet reached its full potential but also shows that afforestation is not a long-term solution for climate change mitigation.