Detecting and measuring emotional responses while interacting with virtual reality (VR), and assessing and interpreting their impacts on human engagement and “immersion,” are both academically and technologically challenging. While many researchers have, in the past, focused on the affective evaluation of passive environments, such as listening to music or the observation of videos and imagery, virtual realities and related interactive environments have been used in only a small number of research studies as a mean of presenting emotional stimuli. This article reports the first stage (focusing on participants' subjective responses) of a range of experimental investigations supporting the evaluation of emotional responses within a virtual environment, according to a three-dimensional (Valence, Arousal, and Dominance) model of affects, developed in the 1970s and 1980s. To populate this three-dimensional model with participants' emotional responses, an “affective VR,” capable of manipulating users' emotions, has been designed and subjectively evaluated. The VR takes the form of a dynamic “speedboat” simulation, elements (controllable VR parameters) of which were assessed and selected based on a 35-respondent online survey, coupled with the implementation of an affective power approximation algorithm. A further 68 participants took part in a series of trials, interacting with a number of VR variations, while subjectively rating their emotional responses. The experimental results provide an early level of confidence that this particular affective VR is capable of manipulating individuals' emotional experiences, through the control of its internal parameters. Moreover, the approximation technique proved to be fairly reliable in predicting users' potential emotional responses, in various affective VR settings, prior to actual experiences. Finally, the analysis suggested that the emotional response of the users, with different gender and gaming experiences, could vary, when presented with the same affective VR situation.