Arsenic is a toxic metal with harmful effects on human health, particularly on cognitive function. Autism Spectrum Disorders (ASDs) are lifelong neurodevelopmental and behavioral disorders manifesting in infancy or early childhood. We used data from 130 children between 2-8 years (65 pairs of ASD cases with age- and sex-matched control), to compare the mean total blood arsenic concentrations in children with and without ASDs in Kingston, Jamaica. Based on univariable analysis, we observed a significant difference between ASD cases and controls (4.03μg/L for cases vs. 4.48μg/L for controls, P < 0.01). In the final multivariable General Linear Model (GLM), after controlling for car ownership, maternal age, parental education levels, source of drinking water, consumption of “yam, sweet potato, or dasheen”, “carrot or pumpkin”, “callaloo, broccoli, or pak choi”, cabbage, avocado, and the frequency of seafood consumption per week, we did not find a significant association between blood arsenic concentrations and ASD status (4.36μg/L for cases vs. 4.65μg/L for controls, P = 0.23). Likewise, in a separate final multivariable GLM, we found that source of drinking water, eating avocado, and eating “callaloo, broccoli, or pak choi” were significantly associated with higher blood arsenic concentrations (all three P < 0.05). Based on our findings, we recommend assessment of arsenic levels in water, fruits, and vegetables, as well as increased awareness among the Jamaican population regarding potential risks for various exposures to arsenic.