Gait is complex, described by diverse characteristics underpinned by widespread central nervous system networks including motor and cognitive functions. Despite this, neural substrates of discrete gait characteristics are poorly understood, limiting understanding of gait impairment in ageing and disease. This structured review aims to map gait characteristics, defined from a pre-specified model reflecting independent gait domains, to brain imaging parameters in older adults. Fifty-two studies of 38,029 yielded were reviewed. Studies showed inconsistent approaches when mapping gait assessment to neural substrates, limiting conclusions. Gait impairments typically associated with brain deterioration, specifically grey matter atrophy and white matter integrity loss. Gait velocity, a global measure of gait control, was most frequently associated with these imaging markers within frontal and basal ganglia regions, and its decline predicted from white matter volume and integrity measurements. Fewer studies assessed additional gait measures or functional imaging parameters. Future studies mapping regional neuroanatomical and functional correlates of gait are needed, including those which take a multi-process network perspective to better understand mobility in health and disease.