Virtual reality (VR) is being implemented by architects recently as an advanced tool to facilitate feedback and discussions. It also provides possibilities to gauge the immersive and experiential attributes of built environments. The felt experiences of the users in a built environment are crucial, as they are associated with the experiential well-being of the occupants. This paper posits that it is essential to investigate the felt experiences that occur in built environments. This paper presents an experimental investigation employing neurophysiological instruments, including EEG, pupillometry, and psychogalvanic sensors, to identify experiences within a VR-built environment. It was determined that the neurophysiological instruments were capable of identifying four distinct emotions experienced during the VR walkthrough by triangulating data from these three sensor systems, despite the presence of numerous emotional processes. This paper argues that neurophysiological sensors can be employed to refine architectural designs by facilitating the study of constructs like experiential well-being, particularly in light of their increasing accessibility.