Andean grasslands (páramos) are highly valued for their role in regional water supply as well as for their biodiversity and large soil carbon stocks. Several Payment for Ecosystem Services (PES) programmes promote either afforestation or alteration of traditional burning regimes under the assumption that these land management strategies will maximize páramo ecosystem services, including carbon storage. However, knowledge of the effects of incentivized land uses is limited. In an evaluation of how afforestation and elimination of burning affect carbon storage at a site in southern Ecuador, we found the highest above-ground biomass carbon levels at afforested sites (99.3–122.0 t C ha−1), while grassland sites reached 23.9 t C ha−1 after 45 years of burn exclusion. Soil carbon storage from 0–20 cm was high across all sites (172.8–201.9 t C ha−1), but was significantly lower with afforestation than with burn exclusion. These findings suggest that, although afforestation is generally favoured when carbon is the primary ecosystem service of interest, grasslands with infrequent burning have important potential as a land management strategy when both above-ground biomass and soil carbon are considered. These results are relevant to the development and adaptation of PES programmes focused on carbon as well as those focused on multiple ecosystem services.