This study evaluated wheat production effects on carbon (C) fractions and soil organic C (SOC) molecular composition of a semiarid Plinthustalf in a trial established near Bethlehem. Treatments applied for 20 consecutive years included two straw management (unburned and burned), three tillage (no-tillage, ploughing and stubble mulch) and two weed control (chemical and mechanical) methods. Samples collected from 0-50mm depth of specific treatment combinations were analyzed for SOC, soil inorganic C (SIC), permanganate oxidizable C (POXC), cold (CWEC) and hot (HWEC) water extractable C, extractable humic substances (CEX), humic acids, fulvic acids (CFA) and SOC functional groups. Humification (HI) and polymerization (PI) indices and alkyl C/O-alkyl C ratios were calculated. No-tillage combinations demonstrated potential to reverse losses of soil C fractions in the 0-50mm layer. Increased POXC, CWEC, CEX and CFA revealed the labile nature of accumulated SOC in no-tillage, suggesting that SOC therein could be rapidly lost if no-tilled soils were again cultivated. Although the HI and PI were not always significant, their decrease in the no-tillage combinations suggest minimal decomposition, which is a benefit in Plinthustalfs with low storage capacity. Positive correlations between SIC and SOC fractions implied that an increase in SOC fractions protected SIC, resulting in its accumulation in no-tillage combinations. Functional groups seemed to mimic fractionated SOC fractions because O-alkyl C decreased with concomitant increase in alkyl, aromatic and carbonyl C. These responses highlighted that no-tillage combinations could be ideal to restore SOC quality in drought-prone agro-ecosystems dominated by sandy soils.