We report a multimodal brain imaging study of 36,678 middle-aged and older adults of European descent, a population sample whose reported alcohol consumption ranged from low (i.e., 1–2 alcohol units per day) to high (i.e., more than 4 alcohol units per day) levels of intake. The scale and granularity of the data provide ample statistical power to identify small associations while accounting for important potential confounds. We observe negative relationships between alcohol intake and global gray and white matter measures, regional GMVs, and WM microstructure indices. The associations we identify are widespread across the brain, and their magnitude increases with the average absolute number of daily alcohol units consumed.