The study presents the effect of soil erosion on vegetation, soil accumulation (SA), SA rate (SAR), soil quality, soil mass, and the soil organic carbon (SOC) pool in Brown Andosols and Histosols in a 24-km area in southwest Iceland. Undisturbed prehistoric soils were distinguished from disturbed historic soils using tephrochronology. Soil erosion has been severe during historic time (last 1135 yr), resulting in the increase of the soil mass deposited in soils covered by vegetation by a factor of 7.3–9.2 and net loss of soil in unvegetated areas. The SAR correlated positively with SOC sequestration. SOC is easily transported and given the extensive accumulation of soil, the net effect of burial and subsequent reduction in decomposition is to increase SOC storage. Nevertheless, the increased accumulation and soil depletion has decreased soil quality, including the SOC, and reduced soil resistance to erosion with the depleted SOC contributing to enrichment of atmospheric CO2. The initial terrestrial disturbance was triggered by anthropogenic land use during the Medieval Warm Period, followed by volcanic activity approximately three centuries later. The combination of harsh climate during the Little Ice Age and drastic anthropogenic perturbations has led to land degradation at a catastrophic scale.