Time series of the natural isotopic composition (2H, 18O) of precipitation and streamwater can provide important insights into ecohydrological phenomena at the catchment scale. However, multi-year, high-frequency isotope datasets are generally scarce, limiting our ability to study highly dynamic short-term ecohydrological processes. Here we present four years of daily isotope measurements in streamwater and precipitation at the Alp catchment (area 47 km2) in Central Switzerland and two of its tributaries (0.7 km2 and 1.6 km2). This data set reveals short-term responses of streamflow isotopes to precipitation events, which otherwise remain obscured when isotopes are sampled weekly or monthly. The observations span the period June 2015 through May 2019, during which several hydrometeorologic extreme events occurred, including a very dry summer in 2018 and below-average snow accumulation in winter 2016/2017. In addition, we provide daily time series of key hydrometeorological variables that, in combination with the isotope data, can be useful for assessing the robustness of ecohydrological models.