Ecosystem services provided by urban forests are increasingly included in municipal-level responses to climate change. However, the ecosystem functions that generate these services, such as biomass carbon (C) uptake, can differ substantially from nearby rural forest. In particular, the scaled effect of canopy spatial configuration on tree growth in cities is uncertain, as is the scope for medium-term policy intervention. This study integrates high spatial resolution data on tree canopy and biomass in the city of Boston, Massachusetts, with local measurements of tree growth rates to estimate the magnitude and distribution of annual biomass C uptake. We further project C uptake, biomass, and canopy cover change to 2040 under alternative policy scenarios affecting the planting and preservation of urban trees. Our analysis shows that 85% of tree canopy area was within 10 m of an edge, indicating essentially open growing conditions. Using growth models accounting for canopy edge effects and growth context, Boston's current biomass C uptake may be approximately double (median 10.9 GgC yr, 0.5 MgC ha yr) the estimates based on rural forest growth, much of it occurring in high-density residential areas. Total annual C uptake to long-term biomass storage was equivalent to <1% of estimated annual fossil CO emissions for the city. In built-up areas, reducing mortality in larger trees resulted in the highest predicted increase in canopy cover (+25%) and biomass C stocks (236 GgC) by 2040, while planting trees in available road margins resulted in the greatest predicted annual C uptake (7.1 GgC yr). This study highlights the importance of accounting for the altered ecosystem structure and function in urban areas in evaluating ecosystem services. Effective municipal climate responses should consider the substantial fraction of total services performed by trees in developed areas, which may produce strong but localized atmospheric C sinks.