The study investigated age-related differences in theory of mind and explored the relationship between this ability, other cognitive abilities, and structural brain measures. A cohort of 106 adults (ages 50-90 years) was recruited. Participants completed tests of theory of mind, verbal and performance intelligence, executive function, and information processing speed and underwent structural magnetic resonance imaging (measurement of whole brain volume, volume of white matter hyperintensities, and diffusion tensor imaging of white matter integrity). Theory of mind ability declined with increasing age, and the relationship between theory of mind and age was fully mediated by performance intelligence, executive function, and information processing speed and was partially mediated by verbal intelligence. Theory of mind performance correlated significantly with diffusion tensor imaging measures of white matter integrity but not with volume of white matter hyperintensities or whole-brain volume. Theory of mind age-related decline may not be independent of other cognitive functions; it may also be particularly susceptible to changes in white matter integrity.