Fluctuations with power-law scaling and long-range temporal correlations (LRTCs) are characteristic to human psychophysical performance. Systems operating in a critical state exhibit such LRTCs, but phenomenologically similar fluctuations and LRTCs may also be caused by slow decay of the system's memory without the system being critical. Theoretically, criticality endows the system with the greatest representational capacity and flexibility in state transitions. Without criticality, however, slowly decaying system memory would predict inflexibility. We addressed these contrasting predictions of the â € criticality' and â € long-memory' candidate mechanisms of human behavioral LRTCs by using a Go/NoGo task wherein the commission errors constitute a measure of cognitive flexibility. Response time (RT) fluctuations in this task exhibited power-law frequency scaling, autocorrelations, and LRTCs. We show here that the LRTC scaling exponents, quantifying the strength of long-range correlations, were negatively correlated with the commission error rates. Strong LRTCs hence parallel optimal cognitive flexibility and, in line with the criticality hypothesis, indicate a functionally advantageous state. This conclusion was corroborated by a positive correlation between the LRTC scaling exponents and executive functions measured with the Rey-Osterrieth Complex Figure test. Our results hence support the notion that LRTCs arise from critical dynamics that is functionally significant for human cognitive performance.