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To fully understand brain processes in the real world, it is necessary to record and quantitatively analyse brain processes during real world human experiences. Mobile electroencephalography (EEG) and physiological data sensors provide new opportunities for studying humans outside of the laboratory. The purpose of this study was to document data from high-density EEG and mobile physiological sensors while humans performed a visual search task both on a treadmill in a laboratory setting and overground in a natural outdoor setting. The data set includes 49 young, healthy participants on an outdoor arboretum path and on a treadmill in a laboratory with a large virtual reality screen. The data provide a valuable research tool for scientists interested in signal processing, electrocortical brain processes, mobile brain imaging, and brain-computer interfaces based on mobile EEG. Given the comparison data between laboratory and real world conditions, researchers can test the viability of new processing algorithms across conditions or investigate changes in electrocortical activity related to behavioural dynamics coded into the data.