Governments worldwide are seeking natural climate solutions that can provide economic stimulus while meeting climate goals. Forests provide essential carbon dioxide (CO2) sequestration services, but their potential may be limited by elevated liana densities often resulting from human disturbance. Here we report the first estimate of liana (Vitis spp.) impacts on CO2 removal rates by trees in temperate Appalachian forests and suggest liana removal with biodiversity safeguards as a potential strategy for improved forest management. Shade-intolerant tree species without lianas removed CO2 20% faster than conspecifics with lianas (p = 0.025). We did not detect significant impacts of liana presence on the CO2 removal rates for shade-tolerant species (p = 0.838). Additionally, the merchantable boles of trees without lianas increased in volume 9% faster annually compared to trees with lianas, for all species (p = 0.003). Our findings indicate that thinning lianas-particularly from light-loving species such as Liriodendron tulipifera-may improve sustainability of forest management and increase carbon storage while mitigating climate change.