Datasets in xlxs, json and csv of soil properties included in the article: Soil organic matter CO2 emissions Soil Gravimetric Moisture Soil temperature Total Cr Total Cu Total Ni Total Zn Total Mn Total Fe pH Mean weight diameter Bulk density Water stable aggregate percentage Water holding capacity Infiltration Sand content Silt content Clay content In this study, the physical and chemical properties of soils under grassland, forest and croplands in the periurban area of Zagreb were investigated in a two-year period. Grasslands consistently exhibited multifunctional benefits, including high organic matter content (4.68% vs. 2.24% in cropland), improved bulk density (1.14 vs. 1.24 g cm−3) and an active carbon cycle indicated by increased CO2 emissions (up to 1403 kg ha−1 day−1 in 2021). Forest soils showed the highest aggregate stability (91.4%) and infiltration (0.0006 cm s−1), while croplands showed signs of structural degradation with the highest bulk density and lowestwater retention (39.9%). Temporal variation showed that grassland was particularly responsive to favourable climatic conditions, with soil porosity and water content improving yearly. Principal component analysis showed that soil structure, biological activity and moisture regulation were linked, with grassland plots favourably positioned along the axes of resilience. The absence of tillage and the presence of permanent vegetation cover contributed to their high capacity for climate and water regulation and carbon sequestration.