Due to the widespread involvement of distributed collaboration triggered by COVID-19, it has become a new trend that has continued into the post-pandemic era. This study investigated collective performance within two collaborative environments (co-located and distancing settings) by assessing inter-brain synchrony patterns (IBS) among design collaborators using functional near-infrared spectroscopy. The preliminary study was conducted with three dyads who possessed 2–3 years of professional product design experience. Each dyad completed two designated design tasks in distinct settings. In the distributed condition, participants interacted through video conferencing in which they were allowed to communicate by verbalization and sketching using a shared digital whiteboard. To prevent the influences of different sketching tools on design outputs, we employed digital sketching for both environments. The interactions between collaborators were identified in three behaviors: verbal only, sketch only, and mixed communication (verbal and sketch). The consequences revealed a higher level of IBS when mixed communication took place in distributed conditions than in co-located conditions. Comparably, the occurrence of IBS increased when participants solely utilized sketching as the interaction approach within the co-located setting. A mixed communication method combining verbalization and sketching might lead to more coordinated cognitive processes when in physical isolation. Design collaborators are inclined to adjust their interaction behaviors in order to adapt to different design environments, strengthen the exchange of ideas, and construct design consensus. Overall, the present paper discussed the performance of virtual collaborative design based on a neurocognitive perspective, contributing valuable insights for the future intervention design that promotes effective virtual teamwork.