While the well log-based lithology classification has been extensively utilized in reservoir characterization, the classification of carbonate sub-facies remains challenging due to the subtle nuances in conventional well-logs. The nuclear magnetic resonance (NMR) log provides extra information of pore size and pore geometry features, improving differentiating carbonate sub-facies. Here we explore the feasibility of using the ratio between NMR longitudinal relaxation time and transverse relaxation time as a potential lithology indicator to determine carbonate sub-facies. We analyzed a series of logging data and corresponding core samples of Arbuckle Group carbonate containing mudstone, packstone, grainstone, incipient breccia, and breccia in northern Kansas for the characteristics of longitudinal relaxation times, transverse relaxation times, and longitudinal over transverse relaxation time ratios. The results show that mudstone, packstone, and grainstone exhibit high, intermediate, and low longitudinal over transverse relaxation time ratios, respectively, while incipient breccia and breccia have a wide range of longitudinal over transverse relaxation time ratios. Furthermore, we evaluated the potential of using longitudinal over transverse relaxation time ratios to classify carbonate sub-facies using multivariate analysis. By adding longitudinal over transverse relaxation time ratios to neutron porosity, total gamma-ray, and conductivity logs as inputs of automated facies classification, the prediction error decreased, especially for incipient breccia. On the contrary, when photoelectric log and computed gamma-ray are also available, adding longitudinal over transverse relaxation time ratios does not improve the accuracy of sub-facies classification. Our results suggest that longitudinal over transverse relaxation time ratio is an independent lithology indicator. However, it cannot replace other logs like gamma-ray and photoelectric logs in classifying carbonate sub-facies. Our study provided valuable evidence and credible elucidation of the importance and physicochemical mechanism of longitudinal over transverse relaxation time ratios, which is essential for deciphering NMR logging data in carbonate reservoirs.