Urbanizing environments alter the hydrological cycle by redirecting stream networks for stormwater and wastewater transmission and increasing impermeable surfaces. These changes thereby accelerate the runoff of water and its constituents following precipitation events, alter evapotranspiration processes, and indirectly modify surface precipitation patterns. Green infrastructure, or low-impact development (LID), can be used as a standalone practice or in concert with gray infrastructure (traditional stormwater management approaches) for cost-efficient, decentralized stormwater management. The growth in LID over the past several decades has resulted in a concomitant increase in research evaluating LID efficiency and effectiveness, but mostly at localized scales. There is a clear research need to quantify how LID practices affect water quantity (i.e., runoff and discharge) and quality at the scale of catchments. In this overview, we present the state of the science of LID research at the local scale, considerations for scaling this research to catchments, recent advances and findings in scaling the effects of LID practices on water quality and quantity at catchment scales, and the use of models as novel tools for these scaling efforts.