Smartphone use in medicine is nearly universal despite a dearth of research assessing utility in clinical performance. We sought to identify and define smartphone use during simulated neuroemergencies. In this retrospective review of a prospective observational single-center simulation-based study, participants ranging from subinterns to attending physicians and stratified by training level (novice, intermediate, and advanced) managed a variety of neurological emergencies. The primary outcome was frequency and purpose of smartphone use. Secondary outcomes included success rate of smartphone use and performance (measured by completion of critical tasks) of participants who used smartphones versus those who did not. In subgroup analyses we compared outcomes across participants by level of training using t-tests and χ2 statistics. One hundred and three participants completed 245 simulation scenarios. Smartphones were used in 109 (45%) simulations. Of participants using smartphones, 102 participants looked up medication doses, 52 participants looked up management guidelines, 11 participants looked up hospital protocols, and 13 participants used smartphones for assistance with an examination scale. Participants found the correct answer 73% of the time using smartphones. There was an association between participant level and smartphone use with intermediate participants being more likely to use their smartphones than novice or advanced participants, 53% versus 29% and 26%, respectively (p < 0.05). Of the intermediate participants, those who used smartphones did not perform better during the simulation scenario than participants who did not use smartphones (smartphone users' mean score [standard deviation] = 12.3 [2.9] vs. nonsmartphone users' mean score [standard deviation] = 12.9 (2.7), p = 0.85). Participants commonly used smartphones in simulated neuroemergencies but use didn't confer improved clinical performance. Less experienced participants were the most likely to use smartphones and less likely to arrive at correct conclusions, and thus are the most likely to benefit from an evidence-based smartphone application for neuroemergencies.