Computational modeling and brain imaging studies suggest that sensitivity to rewards and behaviorist learning principles partly explain smartphone engagement patterns and potentially smartphone dependence. Responses to a questionnaire, and observational measures of smartphone use were recorded for 121 university students. Each participant was also tested with a laboratory task of reward sensitivity and a test of verbal operant conditioning. Twenty-three percent of the sample had probable smartphone addiction. Using multivariate regression, smartphone use, particularly the number of instant messenger services employed, was shown to be significantly and independently predicted by reward sensitivity (a positive relationship), and by instrumental conditioning (a negative relationship). However, the latter association was driven by a subset of participants who developed declarative knowledge of the response-reinforcer contingency. This suggests a process of impression management driven by experimental demand characteristics, producing goal-directed instrumental behavior not habit-based learning. No other measures of smartphone use, including the self-report scale, were significantly associated with the experimental tasks. We conclude that stronger engagement with smartphones, in particular instant messenger services, may be linked to people being more sensitive to rewarding stimuli, suggestive of a motivational or learning mechanism. We propose that this mechanism could underly problem smartphone use and dependence. It also potentially explains why some aspects of smartphone use, such as habitual actions, appear to be poorly measured by technology-use questionnaires. A serendipitous secondary finding confirmed that smartphone use reflected active self-presentation. Our ‘conditioning’ task-induced this behavior in the laboratory and could be used in social-cognition experimental studies.