Farmland abandonment in Mediterranean mid‐mountain areas can lead to the degradation or recovery of soil properties. Typically, after abandonment, fields are covered with shrubs, which hinders livestock grazing and constitutes high wildfire risk. To avoid these negative effects, shrubs are cleared in selected areas. The main objective of this study is to evaluate whether shrub clearing can improve soil quality and enhance carbon sequestration. A case study was conducted in the Leza Valley (La Rioja, Spain), examining five different land uses/management practices in both acid and alkaline soil environments. These included shrubland (control), three shrub clearing sites (managed <5, 15, and 25 years ago), and control pasture (reference). Soil replicates at different depths (0–40 cm) were collected, and physico‐chemical properties were analysed. A theoretical map of potential shrub clearing areas was created, and the potential to accumulate carbon was evaluated. Results showed that shrub clearing increases soil organic carbon and nitrogen, specially in 25‐year clearings. The increases were greater and significant on alkaline environments. The cartographical analysis reveals that 3388 ha can be still cleared in the Leza Valley, which could increase soil organic carbon accumulation by up to 31.6% in 25‐year period. We propose shrub‐clearing as a strategy for enhancing carbon sequestration in Mediterranean mountain areas.