Pollutant nitrogen deposition effects on soil and foliar element concentrations were investigated in acidic and limestone grasslands, located in one of the most nitrogen and acid rain polluted regions of the UK, using plots treated for 8–10 years with 35–140 kg N ha −2 y −1 as NH 4NO 3. Historic data suggests both grasslands have acidified over the past 50 years. Nitrogen deposition treatments caused the grassland soils to lose 23–35% of their total available bases (Ca, Mg, K, and Na) and they became acidified by 0.2–0.4 pH units. Aluminium, iron and manganese were mobilised and taken up by limestone grassland forbs and were translocated down the acid grassland soil. Mineral nitrogen availability increased in both grasslands and many species showed foliar N enrichment. This study provides the first definitive evidence that nitrogen deposition depletes base cations from grassland soils. The resulting acidification, metal mobilisation and eutrophication are implicated in driving floristic changes. Nitrogen deposition causes base cation depletion, acidification and eutrophication of semi-natural grassland soils.