It is important to ensure the ratio of stable and labile soil organic carbon (SOC) compounds in the soil as this influences ecosystem functions and the sustainability of soil management. The aim of this investigation was to determine the changes in SOC compounds and soil quality improvement in Arenosol soil after the conversion of arable land to natural and agricultural land use. The land use types included pine afforestation (PA), uncultivated abandoned land (UAL), unfertilised and fertilised cropland (CLunf, CLf), and unfertilised and fertilised grassland (GRunf, GRf). To assess the lability of organic carbon (OC) compounds, levels of mobile humic substances (MHSs), mobile humic acids (MHAs), mobile fulvic acids (MFAs), active C pool (POXC), and water-soluble C (WEOC) compounds were determined. It was found that faster OC accumulation occurs in PA soil than in CLf, and is somewhat slower in grassland uses (GRf and UAL). As the amount of SOC increased, more MHS formed. A significant increase in their quantity was found in PA (+92.2%) and CRf and UAL (+51.5–52.7%). The application of mineral fertilisers promoted the formation of MHSs in CLf and GRf. PA, GRunf, and GRf soils had more suitable conditions for MHA formation (MHA/MFA > 1.3), whereas CLunf soil contained more MFAs. The POXC pool was insensitive to land-use changes in the Arenosol. After land-use conversion, POXC amounts were significantly (p < 0.05) higher in natural ecosystems (UAL and PA) and fertiliser perennial grasses than in CL. The amount of WEOC increased the most in UAL, PA, and GRf (7.4–71.1%). The sequence of decrease in land use was GRf, UAL, and PA > CLunf, CLf, and GRunf. The decreasing order of the carbon management index (CMI) of different land uses (PA > UAL > GRf > GRunf > Clunf) confirms that faster OC accumulation in Arenosol soil occurred in PA and grassland land uses (GRf and UAL). The values of the carbon lability index (CLI) variation (CLunf > GRunf GRf > UAL > PA) show that in PA, UAL, and GRf land uses, mobile organic matter (OM) forms are relatively less formed, which stabilises OC accumulation in the soil. The CMI showed that UAL and GRf were the most suitable soil uses for Arenosol soils.