This cross-sectional study aimed to determine the use of neuroenhancers, the motivations and factors associated with their use in French and Romanian university students. Students from two universities in France (Rouen and Opal Coast University) and one in Romania (Cluj-Napoca) were asked to complete a self-administered anonymous questionnaire, either online or on paper, about the use of three different categories of substance: Prescription drugs (methylphenidate, modafinil, and beta-blockers), drugs of abuse (alcohol, cannabis, cocaine, and amphetamines), and soft enhancers (coffee, vitamins, caffeine tablets, and energy drinks). In total, 1110 students were included: The users were 2.2% for prescription drugs, 4.3% for drugs of abuse, and 55.0% for soft enhancers. Students used neuroenhancement to stay awake for study (69.3%), to improve concentration (55.5%), to decrease stress (40.9%), and to improve memory (39.6%). Neuroenhancement was considered to meet expectations by 74.4% of users. The factors associated with the use of drugs of abuse were frequent binge drinking (Adjusted Odds Ratio—AOR: 6.49 [95% CI: 2.53–16.6]), smoking (AOR: 5.50 [95% CI: 2.98–10.14]), having a student job (AOR: 2.42 [95% CI 1.13–5.17]), and being male (AOR: 2.23 [95% CI:1.21–4.11]). No significant associations with eating disorders were detected for any of the three categories of substances. University students reported neuroenhancement with prescription drugs, drugs of abuse, and mainly soft enhancers. These substances were used mainly to increase the waking hours. Educational programs in universities seem to be required in order to increase student awareness of the problems caused by neuroenhancements, and to decrease the associated risks by changing students’ attitudes and beliefs.