Humans consistently make suboptimal decisions involving random events, yet the underlying neural mechanisms remain elusive. Using functional MRI and a matching pennies game that captured subjects' increasing tendency to predict the break of a streak as it continued [i.e., the "gambler's fallacy" (GF)], we found that a strong blood oxygen level-dependent response in the left lateral prefrontal cortex (LPFC) to the current outcome preceded the use of the GF strategy 10 s later. Furthermore, anodal transcranial direct current stimulation over the left LPFC, which enhances neuronal firing rates and cerebral excitability, increased the use of the GF strategy, and made the decisions more "sticky." These results reveal a causal role of the LPFC in implementing suboptimal decision strategy guided by false world models, especially when such strategy requires great resources for cognitive control.