Emotions are crucial ingredients of meaningful and memorable tourism experiences. Research methods borrowed from experimental psychology are prime candidates for quantifying emotions while experiences are unfolding. The present article empirically evaluates the methodological feasibility and usefulness of ambulatory recordings of skin conductance responses (SCRs) during a tourism experience. We recorded SCRs in participants while they experienced a roller-coaster ride with or without a virtual reality (VR) headset. Ride elements were identified that related to physical aspects (such as accelerations and braking), to events in the VR environment, and to the physical theming of the roller coaster. VR rides were evaluated more positively than normal rides. SCR time series were meaningfully related to the different ride elements. SCR signals did not significantly predict overall evaluations of the ride. We conclude that psychophysiological measurements are a new avenue for understanding how hospitality, tourism and leisure experiences dynamically develop over time.