In a no-till system (NTS) on naturally acidic soils, surface liming is essential to neutralize soil acidity and increases crop productivity. As a result, the soil organic matter (SOM) pools of the soil surface layers may change, reflecting increased C inputs by crop residues. The objective of this study was to quantify changes in SOM pools and the rate of C sequestration that occur in response to surface liming in a long-term NTS experiment. The experiment was conducted in an Oxisol in southern Brazil. The treatments consisted of the application of 0 or 6 Mg ha -1 of dolomitic lime on the soil surface in 1993 and a reapplication of 0 or 3 Mg ha -1 of dolomitic lime in 2000 to plots with or without the previous lime application. Liming caused total organic C (TOC) accumulation, especially in the 0- to 2.5-cm layer. The amount of TOC stored in the 20-cm layer was 49.9, 52.9, 52.7, and 57.5 Mg ha -1 in the control, 6+0, 0+3, and 6+3 Mg ha -1 treatments, respectively. The levels of particulate organic C (POC) and mineral-associated organic C (MAOC) in the SOM were also enhanced by liming. The increase in POC was directly related ( R2=0.99, P=0.002) to the accumulation of C from crop residues, which was greater in the plots receiving lime treatment. There were positive correlations between TOC and C extractable with hot water, total polysaccharides, and labile polysaccharides. The correlation analysis also demonstrated that TOC was more tightly correlated with POC than with MAOC, indicating a greater influence of the labile fraction on the increase in TOC with surface liming.