Urban green space is purported to offset greenhouse‐gas (GHG) emissions, remove air and water pollutants, cool local climate, and improve public health. To use these services, municipalities have focused efforts on designing and implementing ecosystem‐services‐based “green infrastructure” in urban environments. In some cases the environmental benefits of this infrastructure have been well documented, but they are often unclear, unquantified, and/or outweighed by potential costs. Quantifying biogeochemical processes in urban green infrastructure can improve our understanding of urban ecosystem services and disservices (negative or unintended consequences) resulting from designed urban green spaces. Here we propose a framework to integrate biogeochemical processes into designing, implementing, and evaluating the net effectiveness of green infrastructure, and provide examples for GHG mitigation, stormwater runoff mitigation, and improvements in air quality and health.