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<h4>Objectives</h4>This study assessed the cognitive function of aluminum-exposed participants from an alum mining zone, compared them with unexposed subjects, and aimed to elucidate the effect of aluminum exposure on cognition.<h4>Design</h4>This was a comparative cross-sectional study. Univariate analyses were used to assess the differences between the aluminum-exposed and unexposed groups. Binary logistic regression models were applied to analyze the effect of aluminum exposure.<h4>Setting</h4>The aluminum-exposed participants were included from an alum mining zone and the unexposed subjects were residents from another district without alum-mine-related factories.<h4>Participants</h4>We included 539 aluminum-exposed participants (254 men, 285 women) and 1720 unexposed participants (692 men, 1028 women).<h4>Results</h4>The mean cognition score on Mini-Mental State Examination was 21.34 (± 6.81) for aluminum-exposed participants. The exposed group had 6.77 times (95% confidence interval, 5.09-9.00) more risk of cognitive impairment than the unexposed group, after adjusting for age, sex, and educational level. No statistically significant association was found between exposure duration and cognition.<h4>Conclusions</h4>This study demonstrated a significant association between aluminum exposure and lower cognitive function.