Rapid and accurate prediction of soil organic carbon (SOC) and the carbon fractions that are sensitive to management are vital for evaluating soil fertility and SOC turnover from both long-term and short-term perspectives. This study used 396 soil samples to investigate the individual and combined use of FTIR-PAS and LIBS for both SOC and permanganate oxidizable carbon (POXC) prediction coupled with partial least squares regression (PLSR). The results showed that LIBS from 205 to 899 nm (LIBS-H) was suitable for predicting SOC and POXC, with a coefficient of determination in prediction ( R P 2 ) of 0.68 and 0.73, and a root mean square error in prediction (RMSEP) of 0.57% and 169 mg kg−1, respectively. FTIR-PAS also exhibited good potential for the prediction of SOC and POXC with a slightly poorer performance ( R P 2 of 0.66 and RMSEP of 0.59% for SOC; R P 2 of 0.72 and RMSEP of 171 mg kg−1 for POXC). The prediction ability of SOC was improved by low-level data fusion based on direct concatenation of FTIR-PAS spectra and LIBS spectra at the range of 184–205 nm (LIBS-L), resulting in an R P 2 of 0.72 and an RMSEP of 0.53%. In general, there is good potential for combining FTIR-PAS and LIBS-L to improve the SOC prediction. Both FTIR-PAS and LIBS-H can be applied for individual prediction of SOC and POXC. In addition, FTIR-PAS offers the advantages of reduced complexity in the modeling and easier sample preparation.
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