In this study, we explore the use of unsteady transit time distribution (TTD) theory to model solute transport in biofilters, a popular form of nature-based or “green” storm water infrastructure (GSI). TTD theory has the potential to address many unresolved challenges associated with predicting pollutant fate and transport through these systems, including unsteadiness in the water balance (time-varying inflows, outflows, and storage), unsteadiness in pollutant loading, time-dependent reactions, and scale-up to GSI networks and urban catchments. From a solution to the unsteady age conservation equation under uniform sampling, we derive an explicit expression for solute breakthrough during and after one or more storm events. The solution is calibrated and validated with breakthrough data from 17 simulated storms at a field-scale biofilter test facility in Southern California, using bromide as a conservative tracer. TTD theory closely reproduces bromide breakthrough concentrations, provided that lateral exchange with the surrounding soil is accounted for. At any given time, according to theory, more than half of the water in storage is from the most recent storm, while the rest is a mixture of penultimate and earlier storms. Thus, key management endpoints, such as the pollutant treatment credit attributable to GSI, are likely to depend on the evolving age distribution of water stored and released by these systems.