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The arsenic (As) methylation capacity is an important determinant of susceptibility to As-related diseases. Total As (TAs) or inorganic As (iAs) was reported to associated with As methylation capacity. We measured urinary concentrations of iAs, monomethylarsonic acid (MMA), and dimethylarsinic acid (DMA) by using HPLC-HG-AFS and calculated the primary methylation capacity index (PMI) and secondary methylation capacity index (SMI) in 209 university students in Hefei, China, a non-As endemic area. Volunteers were given a standardized questionnaire asking about their sociodemographic characteristics. Bayesian kernel machine regression (BKMR) analysis was used to estimate the association of lnTAs and lniAs levels with methylation indices (ln%MMA, ln%DMA, lnPMI, lnSMI). The median concentrations of iAs, MMA, and DMA were 1.22, 0.92, and 12.17 μg/L, respectively; the proportions of iAs, MMA, and DMA were 8.76%, 6.13%, and 84.84%, respectively. Females had higher %DMA and lower %MMA than males. The combined levels of lnTAs and lniAs showed a decrease in the changes in ln%DMA and lnSMI. With regard to the single exposure level, the lnTAs showed positive correlations with ln%DMA, lnPMI, and lnSMI when lniAs was set at a specific level, while lniAs showed negative correlations with ln%DMA, lnPMI, and lnSMI when lnTAs was set at a specific level; all the dose-response relationships were nonlinear. Our results suggested that combined levels of TAs and iAs play an important role in reducing As methylation capacity, especially iAs, and the reduction only occurs when TAs and iAs are present up to a certain combined level. [ABSTRACT FROM AUTHOR]