The study of cognitive processes underlying natural behaviors implies departing from computerized paradigms and artificial experimental probes. The present study aims to assess the feasibility of capturing neural markers (P300 ERPs) of cognitive processes evoked in response to the identification of task-relevant objects embedded in a real-world environment. To this end, EEG and eye-tracking data were recorded while participants attended stimuli presented on a tablet and while they searched for books in a library. Initial analyses of the library data revealed that P300-like features shifted in time. A Dynamic Time Warping analysis confirmed the presence of P300 ERP in the library condition. Library data were then lag-corrected based on cross-correlation coefficients. Together, these approaches uncovered P300 ERP responses in the library recordings. These findings highlight the relevance of scalable experimental designs, joint brain and body recordings, and template-matching analyses to capture cognitive events during natural behaviors.