The study aimed to evaluate the relationships between air pollutants and risk of magnetic resonance imaging (MRI)-defined brain infarcts (BI). We used data from routine health examinations of 1,400,503 participants aged ≥18 years who underwent brain MRI scans in 174 cities in 30 provinces in China in 2018. We assessed exposures to particulate matter (PM)_2.5, PM₁₀, nitrogen dioxide (NO₂), and carbon monoxide (CO) from 2015 to 2017. MRI-defined BI was defined as lesions ≥3 mm in diameter. Air pollutants were associated with a higher risk of MRI-defined BI. The odds ratio (OR) (95% CI) for MRI-defined BI comparing the highest with the lowest tertiles of air pollutant concentrations was 2.00 (1.96–2.03) for PM_2.5, 1.68 (1.65–1.71) for PM₁₀, 1.58 (1.55–1.61) for NO₂, and 1.57 (1.54–1.60) for CO. Each SD increase in air pollutants was associated with 16–42% increases in the risk of MRI-defined BI. The associations were stronger in the elderly subgroup. This is the largest survey to evaluate the association between air pollution and MRI-defined BI. Our findings indicate that ambient air pollution was significantly associated with a higher risk of MRI-defined BI.