The impact of hillslope vegetation restoration on the distribution and variability of carbon and water storage was studied across two catenary sequences of soils in the Liudaogou watershed of China’s Loess Plateau. Soil organic carbon storage (SOCS) under different land uses in the two catenas decreased significantly in the upper soil layers (<50 cm) but was relatively stable in the deeper soil layers (>50 cm). However, soil inorganic carbon storage (SICS) in the two catenas fluctuated (two maxima) with increasing soil depth. There was no significant difference of SOCS within the 200 cm soil profile between forestlands (FO) and grasslands (GR) at the catenary scale (p > 0.05). However, SICS in the 0–200 cm soil profile differed markedly between FO and GR (p < 0.05) in both catenas due to different degrees of root-facilitated CaCO₃ redistribution. Based on the coefficient of variance (CV), soil water storage (SWS) was divided into three layers: active layer (0–100 cm, CV = 20%–30%), subactive layer (100–200 cm, CV = 10%–20%), and stable layer (200–500 cm, CV < 10%). The SWS in the 0–500 cm soil profile was slightly higher in GR than in FO on the two slopes because of the higher water consumption under tree plantation than native grasses. SOCS, SICS, and SWS can be predicted by multiple regression equations using different soil properties. The study demonstrated that SOCS, SICS, and SWS respond differently to vegetation restoration at the catenary scale, which must be taken into account for improving ecosystem model predictions of soil carbon and water fluxes in sloping lands.