Introduction: How education affects the relationship between sedentary behavior and cognitive function remains unclear. The aim of this study was to investigate the relationship between mentally active sedentary behavior and cognitive function in rural older Chinese across different levels of education. Methods: Data from 517 participants aged 60 years and older in rural China at baseline, 4 weeks, 8 weeks, 6 months, 12 months, and 24 months were analyzed. Univariate analysis was carried out using descriptive statistical techniques and bivariate analysis was performed using linear mixed effects models. Results: Total mentally active sedentary behavior time and playing cards/mahjong time were significantly associated with global cognition (0.25 points [95% CI, 0.15–0.35], p < 0.001; 0.27 points [95% CI, 0.16–0.37], p < 0.001, respectively), the attention dimension (0.07 points [95% CI, 0.01–0.12], p = 0.025; 0.08 points [95% CI, 0.02–0.14], p = 0.011, respectively), and the memory dimension (0.20 points [95% CI, 0.13–0.26], p < 0.001; 0.18 points [95% CI, 0.12–0.25], p < 0.001, respectively). Such associations were more pronounced in illiterate participants. Conclusion: Our study suggested a positive association between mentally active sedentary behavior and cognitive function, with the association being more pronounced among illiterate older adults compared to the relatively well-educated. Future cognitive interventions should focus more on mentally active behavior. In addition, education-specific intervention strategy may be considered in cognitive interventions.

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