Description: Form and function are two major characteristics of hydrological systems. While form summarizes the structure of the system, function represents the hydrological response. Little is known about how these characteristics evolve and how form relates to function in young hydrological systems. We investigated how form and function evolve during the first millennia of landscape evolution. We analyzed two hillslope chronosequences in glacial forelands, one developed from siliceous and the other from calcareous parent material. Variables describing hillslope form included soil physical properties, surface, and vegetation characteristics. Variables describing hydrological function included soil water response times, soil water storage, drainage, and dominant subsurface flow types. We identified links between form and hydrological function via cluster analysis. Clusters identified based on form were compared in terms of their hydrological functioning. The comparison of the two different parent materials shows how strongly landscape evolution is controlled by the underlying geology. Soil pH appears to be a key variable influencing vegetation, soil formation and subsequently hydrology. At the calcareous site, the high buffering capacity of the soil leads to less soil formation and fast, vertical subsurface water transport dominates the water redistribution even after more than 10,000 years of landscape evolution. At the siliceous site, soil acidification results in accumulation of organic material, a high water storage capacity, and in podsolization. Under these conditions water redistribution changes from vertical subsurface water transport at the young age classes to water storage in the organic surface layer and lateral subsurface water transport within 10,000 years.