To provide a sound understanding of the sources, pathways, and residence times of groundwater water in alluvial river-aquifer systems, a combined multitracer and modeling experiment was carried out in an important alluvial drinking water wellfield in Switzerland. 222Rn, 3H/3He, atmospheric noble gases, and the novel 37Ar-method were used to quantify residence times and mixing ratios of water from different sources. With a half-life of 35.1 days, 37Ar allowed to successfully close a critical observational time gap between 222Rn and 3H/3He for residence times of weeks to months. Covering the entire range of residence times of groundwater in alluvial systems revealed that, to quantify the fractions of water from different sources in such systems, atmospheric noble gases and helium isotopes are tracers suited for end-member mixing analysis. A comparison between the tracer-based mixing ratios and mixing ratios simulated with a fully-integrated, physically-based flow model showed that models, which are only calibrated against hydraulic heads, cannot reliably reproduce mixing ratios or residence times of alluvial river-aquifer systems. However, the tracer-based mixing ratios allowed the identification of an appropriate flow model parametrization. Consequently, for alluvial systems, we recommend the combination of multitracer studies that cover all relevant residence times with fully-coupled, physically-based flow modeling to better characterize the complex interactions of river-aquifer systems.