The context menu only has the option to add a complete file type. Online, I also only find ways to add complete file types to lfs.
From the look of it, it seems that it should be possible to use more specific patterns for folders / subfolders / filetypes, but I can't get that to work; lfs only ever works if it's really only a "*.mytype" declaration.
In some cases, I really want to track some specific folders and files in LFS while others of the same filetype should live in regular git land. Specifically, the ".asset" extension in Unity is used for a ton of things ranging from simple, text-readable ScriptableObjects (which should live in git land) to texture arrays with a size of several hundred MB (that's for LFS then).
Edit/Addendum: seems I can workaround by having a "fake" extension like ".lfs.asset", which I can manually add to the .gitattributes file. Also, I figured that sometimes (not always) directory pathes seem to work, as long as they don't contain any spaces and thus don't need any "" or '' in the .gitattributes file... but that's more of a workaround than a real solution, so please chime in if you know more!