In this quasiexperimental study, we examined whether the introduction of an age-friendly transportation policy—free bus passes for older adults—increased public transport use and in turn affected cognitive function among older people in England. Data came from 7 waves (2002–2014) of the English Longitudinal Study of Ageing (n = 17,953), which measured total cognitive function, memory, executive function, and processing speed before and after the bus pass was introduced in 2006. The analytical strategy was an instrumental-variable approach with fixed effects, which made use of the age-eligibility criteria for free bus passes and addressed bias due to reverse causality, measurement error, and time-invariant confounding. Eligibility for the bus pass was associated with a 7% increase in public transport use. The increase in public transportation use was associated with a 0.346 (95% confidence interval: 0.017, 0.674) increase in the total cognitive function z score and with a 0.546 (95% confidence interval: 0.111, 0.982) increase in memory z score. Free bus passes were associated with an increase in public transport use and, in turn, benefits to cognitive function in older age. Public transport use might promote cognitive health through encouraging intellectually, socially, and physically active lifestyles. Transport policies could serve as public health tools to promote cognitive health in aging populations.