ABSTRACT As GIS progressively permeates our everyday lives, it becomes increasingly significant to incorporate emotional factors into the design and use of GIS technologies. While existing methods such as self‐report and AI‐enhanced techniques prevail in collecting emotional factors, they often miss real‐time emotional nuances and synchronization with geographically referenced and other accompanying data. To bridge this gap, we introduce “Neural Sensing,” a novel approach that combines Electroencephalogram (EEG) with GIS technologies to quantitatively measure emotional responses to places. This approach offers a unique lens to understand human dynamics in a hybrid physical–virtual realm, especially by delving into our mental worlds. To demonstrate the utility of Neural Sensing, we have designed a pilot empirical study to analyze emotional reactions to geographical environments. This approach broadens the domain of GIS methodologies from remote sensing and social sensing to a neural sensing approach. Through this study, we underscore the importance of the mental dimension of the hybrid physical–virtual world and encourage GIScientists to emphasize human experiences and feelings in GIS analyses.