Given the rapid advancements in neuroscience and its growing involvement in legal proceedings, in this paper, we aim to address the question of whether and to which extent Greek legislation could be revisited in the light of the most recent neuroscientific discoveries. “Reading” the human cognitive and emotional functions by modern neuroscientific technology is relevant to a number of Greek legal provisions, an overview of which is presented in this paper. In the first chapter, we describe the general framework that governs an adult’s capacity of will, taking into consideration the constitutional aspect, the civil law’s approach and some special topics concerning medical law and research, with the aim to examine how these issues could be illuminated with a neuroscientific perspective. The second chapter is exclusively dedicated to criminal law, in an effort to evaluate the potential influence of neuroscience on the Greek criminal justice system. The penal legislation concerning the assessment of criminal responsibility, the evaluation of the sentence, and the admissibility of neuroscientific techniques in criminal Courts, as well as some special issues concerning juvenile offenders and crime prevention are presented. Finally, a unique Greek case where the use of a lie detector was permitted in the context of a criminal trial is cited and briefly analysed. This overview leads to conclude that although the Greek legal system refers extensively to situations of interest for neurolaw, the acceptance of neuroscientific methods for determining the cognitive or mental status of persons involved in civil, medical and criminal relationships is rarely considered as important. However, the aforementioned judicial step towards the acceptance of these methods in criminal settings, as well as the innovative spirit that the Greek legislator shows in regulating biomedical matters during the last decades, lead to consider that a revision of the Greek legislation in the light of new neuroscience, should not be excluded for the future. Providing more information on neurolaw and its expected benefits could be, perhaps, the best motivation for taking action in this promising field.