Information and communication services have become ubiquitous in our everyday life and, in turn, research on Ubiquitous Information Systems (UIS) has received increasing attention. UIS services can elicit both negative and positive emotions, which are not necessarily perceived consciously by individuals but which may still have an impact on predictors and outcomes of UIS service use. Due to the limita- tions of psychological self-reports in uncovering these automatic cognitive pro- cesses, the current work investigates emotional stimuli of UIS services with neu- rophysiological data. In particular, we choose electrodermal activity as an indica- tor of physiological arousal and assess its utility for the design and use of UIS ser- vices. To account for the neurophysiological nature of electrodermal activity and to investigate its value in relation to established self-report instruments, we integrate the stimulus-organism-response paradigm with a two-systems view of cognitive processing. Against the background of this theoretical framework, we hypothesize relationships between breakdown events of UIS services (the emotional stimuli), physiological arousal and perceived ease of use (manifestations of the organism’s automatic and inferential cognitive processes), and task performance (the response of the organism). We also consider physiological learning processes related to generalization effects. In order to test the hypotheses, we use empirical data from two studies. Results indicate that electrodermal activity is a useful measure for the design and use of UIS services, even though generalization effects can reduce its reliability. Moreover, we demonstrate that electrodermal activity is related to perceived ease of use and task performance. We finally discuss the theoretical and practical implications of our results, examine the limitations of the current work and outline future research.