Background: Both physical activity (PA) and sedentary behavior (SB) are important factors for healthy ageing. This systematic review aimed to determine the association of objectively assessed (instrumented) PA and SB with global cognitive function in older adults. Methods: PubMed, Embase, the Cochrane Library (via Wiley), CINAHL, PsychINFO, and SPORTDiscus (via EBSCO) were searched from inception to June 21, 2020 for articles that described associations of objectively assessed PA/SB with global cognitive function in older adults aged 60 years and older. Results were synthesized using an effect direction heat map and albatross plots portrayed estimated effect sizes (standardized regression coefficients (βs)), which were summarized in boxplots. Results: In total, 45 articles were included representing a total of 15,817 older adults (mean/median age ranged from 65 to 88 years; 49.5% female). Longitudinal studies (n = 7) showed that higher moderate-to-vigorous and light PA (MVPA and LPA, respectively) and lower SB were associated with better global cognitive function. Standardized βs of cross-sectional studies (n = 38) showed that lower SB (median [IQR], β = 0.078 [0.004-0.184] and higher LPA (β = 0.096 [0.046-0.188]), activity counts (β = 0.131 [0.049-0.224]), number of steps (β = 0.155 [0.096-0.246]), MVPA (β = 0.163 [0.069-0.285]) and total PA (TPA) (β = 0.174 [0.147-0.255]) were associated with better global cognitive function. Conclusions: Higher PA and lower SB are associated with better global cognitive function in older adults. The greatest estimated effect sizes were found for moderate-to-vigorous and TPA, suggesting that greater duration of any PA, and high intensity PA could be most beneficial for global cognitive function.