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Exposure to dust particles enriched with arsenic (As) is a significant health threat for populations living in Southeast Asian megacities. The mineralogical composition of dust particles is the key factor that controls the retention and release of As. This study investigated the degree of metal(oid)s pollution (As, Ca, Fe, K, Ga, Rb, Sr, Ti, V, Y, and Zr) in road dust of Dhaka city, Bangladesh. Enrichment factor and geoaccumulation index suggested that the road dust was heavily enriched with As, which triggers a comprehensive investigation of its controlling mechanisms and potential health risks by combining physicochemical and mineralogical information with multivariate analysis and a simulated probabilistic risk estimation model. Alkaline road dust (pH 1:5 ranges from 8.02 to 10.34) in Dhaka city was found to have significant enrichment of As. Dust alkalinity was possibly controlled by the presence of carbonate minerals, such as calcite. Quartz was identified as the dominant mineral phase followed by magnesium carbon arsenide (MgCAs 2 ). Carbonate mineral driven alkaline pH conditions in road dust would potentially trigger the release and mobilization of As to the environment. However, organic complexation can stabilize As on particle surfaces. Monte Carlo simulation-based health risk forecast suggested that the probability of As associated cancer risk has greatly exceeded the threshold value of 1E-4 for adults and children, and children are more vulnerable than adults. According to sensitivity analysis, the concentration of As and exposure duration (ED) posed the most significant impact (>58%) on risk estimation., (Copyright © 2021 Elsevier Ltd. All rights reserved.)