While place-based methods are increasingly being used to explore why place matters for health, how places matters for mental health and psychological wellness is less understood. Overall, approaches that consider community, environmental, and neighborhood-level factors have been taken up to a lesser extent by psychologists. Yet methods that situate human behavior within a spatial context have the potential to expand psychological and interdisciplinary inquiry aimed at improving mental and cognitive health. This article presents a brief overview of one type of mobile method, the go-along walk, that can be used with a variety of technologies and complementary methods to better understand how individuals respond to places and environmental stimuli, including place-based exposures. Implications for broadening the range of research questions and translational applications are discussed.