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Refereed/Peer-reviewed The relationships between cognitive function and each of physical activity, sleep and sedentary behaviour in older adults are well documented. However, these three “time use” behaviours are co-dependent parts of the 24-hour day (spending time in one leaves less time for the others), and their best balance for cognitive function in older adults is still largely unknown. This systematic review summarises the existing evidence on the associations between combinations of two or more time-use behaviours and cognitive function in older adults. Embase, Pubmed, PsycInfo, Medline and Emcare databases were searched in March 2020 and updated in May 2021, returning a total of 25,289 papers for screening. A total of 23 studies were included in the synthesis, spanning >23,000 participants (mean age 71 years). Findings support previous evidence that spending more time in physical activity and limiting sedentary behaviour is broadly associated with better cognitive outcomes in older adults. Higher proportions of moderate-vigorous physical activity in the day were most frequently associated with better cognitive function. Some evidence suggests that certain types of sedentary behaviour may be positively associated with cognitive function, such as reading or computer use. Sleep duration appears to share an inverted U-shaped relationship with cognition, as too much or too little sleep is negatively associated with cognitive function. This review highlights considerable heterogeneity in methodological and statistical approaches, and encourages a more standardised, transparent approach to capturing important daily behaviours in older adults. Investigating all three time-use behaviours together against cognitive function using suitable statistical methodology is strongly recommended to further our understanding of optimal 24-hour time use for brain function in aging.