Use of 'smart drugs' among UK students is described in frequent media reports as a rapidly increasing phenomenon. This article reports findings from the first large-scale survey of pharmacological cognitive enhancement (PCE) among students in the UK and Ireland. Conducted from February to September 2012, a survey of a convenience sample of 877 students measured PCE prevalence, attitudes, sources, purposes and ethics. Descriptive and logistic regression statistical methods were used to analyse the data. Lifetime prevalence of PCE using modafinil, methylphenidate or Adderall was under 10%, while past regular and current PCE users of these substances made up between 0.3%-4% of the survey population. A substantial majority of students was unaware of and/or uninterested in PCE; however about one third of students were interested in PCE. PCE users were more likely to be male, British and older students; predictors of PCE use included awareness of other students using PCEs, ADHD symptomatology, ethical concerns, and alcohol and cannabis use. The survey addresses the need for better evidence about PCE prevalence and practices among university students in the UK. We recommend PCE-related strategies for universities based on the survey findings.