AbstractLateral subsurface stormflow (SSF) is the most important runoff generation mechanism for most hillslopes in temperate climates. It is influenced by pedological, biological, and topographic factors that change during landscape evolution, but so far little is known about how SSF changes over long‐time scales. Therefore, we conducted sprinkling experiments on a silicate and carbonate moraine chronosequence in the Swiss Alps. Each chronosequence consisted of four moraines ranging between a couple of decades and ∼13,500 years in age. On each moraine, we installed three plots and measured shallow SSF in a trench. We added tracers (δ2H and NaCl) to the sprinkling water to identify mixing and flow pathways in the subsurface. The coarse and drainable sediments on the young moraines provoked more frequent and larger SSF responses than for the old moraines. There was no SSF during the sprinkling experiments on the older moraines at the calcareous study area, but SSF occurred during larger natural rainfall events. The pre‐event water fractions in SSF were higher for the old moraines than the young moraines due to the increase in silt, clay, and soil organic matter content, and subsequent increase in the amount of water stored in the soil. The results of this study suggest that soil and vegetation development affect SSF characteristics and help—together with the results for overland flow (companion paper; Maier & van Meerveld, 2021, https://doi.org/10.1029/2021WR030221)—to improve hydrological models and our understanding of the changes in near‐surface runoff generation processes during the first millennia of landscape evolution in Alpine areas.