While walking in our natural environment, we continuously solve additional cognitive tasks. This increases the demand of resources needed for both the cognitive and motor systems, resulting in Cognitive-Motor Interference (CMI). While it is well known that a performance decrease in one or both tasks can be observed, little is known about human brain dynamics underlying CMI during dual-task walking. Moreover, a large portion of previous investigations on CMI took place in static settings, emphasizing the experimental rigor but overshadowing the ecological validity. To address these problems, we developed a dual-task walking scenario in virtual reality (VR) combined with Mobile Brain/Body Imaging (MoBI). We aimed at investigating how brain dynamics are modulated during natural overground walking while simultaneously performing a visual discrimination task in an ecologically valid scenario. Even though the visual task did not affect performance while walking, a P3 amplitude reduction along with changes in power spectral densities (PSDs) during dual-task walking were observed. Replicating previous results, this reflects the impact of walking on the parallel processing of visual stimuli, even when the cognitive task is particularly easy. This standardized and easy to modify VR-paradigm helps to systematically study CMI, allowing researchers to control the complexity of different tasks and sensory modalities. Future investigations implementing an improved virtual design with more challenging cognitive and motor tasks will have to investigate the roles of both cognition and motion, allowing for a better understanding of the functional architecture of attention reallocation between cognitive and motor systems during active behavior.