Human’s uncertain decision-making involves choices of risk (with known probabilities) and ambiguity (with unknown probabilities). For risky and ambiguous decision-making processes, neural differences are rarely exhibited. To clarify the causal role of the right dorsolateral prefrontal cortex (DLPFC) in uncertain situations, we used transcranial direct current stimulation (tDCS) to demonstrate the involvement of the right DLPFC in decisions involving risk and ambiguity. Participants received either anodal or cathodal tDCS at 1.5 mA or sham stimulation over the right DLPFC and subsequently undertook tasks of risk and ambiguity. The results revealed that a preference for ambiguity could be measurably increased in individuals through anodal stimulation, but no significant differences were observed in the preferences for risky choices among groups. These findings suggest that different neural mechanisms underlie risky and ambiguous decisions because the right DLPFC primarily affects ambiguous behavior.