Background: Ambient particulate matter of ≤2.5 μm in diameter (PM2.5) is named as a risk factor for cerebrovascular diseases. This investigation aimed to evaluate the impact of ambient air pollution with PM2.5 on stroke occurrence. Methods: The study was performed in Kaunas, Lithuania, from 2010 to 2022. The daily numbers of ISs, subarachnoid hemorrhages (SAHs), and intracerebral hemorrhages (ICHs) were obtained from the Kaunas Stroke Register. The association between stroke occurrence and PM2.5 exposure was assessed by time- and seasonally stratified Poisson regression. Results: Among middle-aged persons, 3377 had a stroke, of which 2686 (79.5%) had an IS, 469 (13.9%) had an ICH, and 222 (6.6%) had SAH. The relative risk (RR) of SAH was increased by 1.7% with an increase in daily PM2.5 by 1 μg/m3 on the same day and at a lag of 1 day, and by 2.2% with an increase in mean PM2.5 concentration at a lag 0–1 days by 1 μg/m3. The RR of having a SAH was increased by 0.7% with an increase in daily PM2.5 by 1 μg/m3 on the same day. Conclusions: Significant associations between stroke occurrence and air pollution with PM2.5 were found in the SAH and HS patients, and only in middle-aged subjects.