Background: The effects of anodal transcranial direct-current stimulation (tDCS) on endurance exercise performance are not yet fully understood. Different stimulated areas and low focality of classical tDCS technique may have led to discordant results. Purpose: This study investigated the effect of a bilateral anodal high-definition tDCS (HD-tDCS) of the dorsolateral prefrontal cortex on the cycling time-trial (TT) performance and physiological and perceptual response at moderate intensity in elite cyclists. Methods: A total of 8 elite cyclists (maximal oxygen consumption: 72.2 [4.3] mL·min−1·kg−1) underwent in a double-blind, counterbalanced, and randomized order the experimental treatment (HD-tDCS) or control treatment (SHAM). After 20 minutes of receiving either HD-tDCS on the dorsolateral prefrontal cortex (F3 and F4) or SHAM stimulation, the participants completed a constant-load trial (CLT) at 75% of the second ventilatory threshold. Thereafter, they performed a simulated 15-km TT. The ratings of perceived exertion, heart rate, cadence,  oxygen consumption, and respiratory exchange ratio were recorded during the CLT; the ratings of perceived exertion and heart rate were recorded during the TT. Results: The total time to complete the TT was 1.3% faster (HD-tDCS: 1212 [52] s vs SHAM: 1228 [56] s; P = .04) and associated with a higher heart rate (P < .001) and a tendency toward higher mean power output (P = .05). None of the physiological and perceptual variables measured during the CLT highlighted differences between the HD-tDCS and SHAM condition. Conclusions: The findings suggest that bilateral HD-tDCS on the dorsolateral prefrontal cortex improves cycling TT performance without altering the physiological and perceptual response at moderate intensity, indicating that an upregulation of the prefrontal cortex could enhance endurance exercise performance.