Human actions compromise the many life-supporting functions provided by the freshwater cycle. Yet, scientific understanding of anthropogenic freshwater change and its long-term evolution is limited. Here, using a multi-model ensemble of global hydrological models, we estimate how, over a 145-year industrial period (1861–2005), streamflow and soil moisture have deviated from pre-industrial baseline conditions (defined by 5th–95th percentiles, at 0.5° grid level and monthly timestep over 1661–1860). Comparing the two periods, we find an increased frequency of local deviations on ~45% of land area, mainly in regions under heavy direct or indirect human pressures. To estimate humanity’s aggregate impact on these two important elements of the freshwater cycle, we present the evolution of deviation occurrence at regional to global scales. Annually, local streamflow and soil moisture deviations now occur on 18.2% and 15.8% of global land area, respectively, which is 8.0 and 4.7 percentage points beyond the ~3 percentage point wide pre-industrial variability envelope. Our results signify a substantial shift from pre-industrial streamflow and soil moisture reference conditions to persistently increasing change. This indicates a transgression of the new planetary boundary for freshwater change, which is defined and quantified using our approach, calling for urgent actions to reduce human disturbance of the freshwater cycle.