Cropland (CRL) abandonment is a worldwide phenomenon of land use change with significant impacts on agro‐ecosystems. This research attempts to deepen the analysis of the positive and negative effects arising by focusing on the changes in soil properties and the amount and composition of soil particles detached after several periods of rainfall and the resulting exported sediment that occurs in abandoned areas with natural revegetation compared to CRL. The study was carried out in an agroforestry catchment with a temperate climate, on which CRL and abandoned land with natural vegetation were compared. The soil was sampled along two representative hillslopes integrating elements of the landscape and land use/land covers. Sediments were collected after seven periods in which flood events were recorded during the period July 2016 to December 2017, using artificial‐lawn mats. Soil and sediment composition (texture, soil organic carbon [SOC] and nutrients [total nitrogen and total phosphorous]) under both land uses were assessed and compared and related to rainfall characteristics using principal component analysis. Nutrient enrichment factors in the sediments compared to soils were also evaluated. The results highlight that after abandonment, SOC increased significantly, reaching contents almost three times higher than in CRL. Consequently, soil erodibility decreased, resulting in substantially lower sediment generation after erosive rainfall events. On average, sediment generation was three times lower in abandoned areas than in CRL, despite their steeper slopes. Soil total nitrogen also increased on abandoned lands, reaching values about twice as high as those in CRL. However, total phosphorous content was almost twice as high in CRL than in abandoned land posing a potential risk for water due to higher erosion rates recorded in CRL. The results confirmed the association of phosphorous with smaller particles and also demonstrated the total phosphorous‐SOC link in abandoned land. Furthermore, the effect of rainfall intensity on phosphorous mobilisation was confirmed, whilst nitrogen losses were mainly related to the total amount of rainfall recorded. In a scenario of increasing extreme precipitation, both total amount and increased precipitation intensity may exacerbate water pollution problems following nutrient loss in cultivated areas. This research contributes to identifying the impacts on agroforestry systems within the current context of converting natural areas into cultivated land, whilst in other regions revegetated natural areas are developed from abandoned agricultural land.