The aim of this study is to provide new knowledge on the effect of willow on hillslope hydrology at a slope scale. Soil moisture and matric suction were monitored in situ under willow-vegetated and fallow ground covers on a small-scale hillslope in Northeast Scotland for 21 months. The retrieved time series were analysed statistically to evaluate whether the dynamics of soil moisture and matric suction changed with the hillslope zone (i.e., toe, middle, and crest) under the two ground covers. The effect of air temperature and rainfall on the dynamics of soil moisture and matric suction, as well as the relationship between the two soil-water variables, under both ground covers, were also investigated by analysing the cross-correlation between time series. The results of 21 months of monitoring showed that willow contributed substantially to reduce soil moisture and to increase matric suction with respect to fallow soil. Additionally, willow-vegetated soil exhibited higher water retention and moisture buffering capacity than fallow soil. The effect of willow was highest at the hillslope toe due to a denser vegetation cover present within this zone. Both air temperature and rainfall had a strong effect on soil moisture and matric suction. However, the effect of air temperature was more consistent and easier to interpret than that of rainfall. Soil moisture and matric suction were shown to have a complex relationship and the soil water characteristic curve for vegetated soil requires further research. This study provides novel, field-based information supporting the positive effect of willow on hillslope hydrology. The results gathered herein will undoubtedly enhance the confidence of using woody vegetation in Nature-based Solutions (NBS) against geo-climatic hazards.