High psychopathy is characterized by untruthfulness and manipulativeness. However, existing evidence on higher propensity or capacity to lie among non-incarcerated high-psychopathic individuals is equivocal. Of particular importance, no research has investigated whether greater psychopathic tendency is associated with better ‘trainability’ of lying. An understanding of whether the neurobehavioral processes of lying are modifiable through practice offers significant theoretical and practical implications. By employing a longitudinal design involving university students with varying degrees of psychopathic traits, we successfully demonstrate that the performance speed of lying about face familiarity significantly improved following two sessions of practice, which occurred only among those with higher, but not lower, levels of psychopathic traits. Furthermore, this behavioural improvement associated with higher psychopathic tendency was predicted by a reduction in lying-related neural signals and by functional connectivity changes in the frontoparietal and cerebellum networks. Our findings provide novel and pivotal evidence suggesting that psychopathic traits are the key modulating factors of the plasticity of both behavioural and neural processes underpinning lying. These findings broadly support conceptualization of high-functioning individuals with higher psychopathic traits as having preserved, or arguably superior, functioning in neural networks implicated in cognitive executive processing, but deficiencies in affective neural processes, from a neuroplasticity perspective.