Captain Disillusion said it wasn’t possible to delete materials with no users. But I discovered that you can! In the Outliner, change the Display Mode to “Blender File” and it’ll show you everything associated with your file—objects, meshes, materials, etc. You can right click and “Delete” a material. Just a (safer) alternative to save and revert, giving you a little more control. Plus it was fun to dig in and see the hierarchy of the file and the relationship and cardinality of its entities.
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I probably would not go that route. Like you said it is safer to save and revert. I would think deleting from blender file would require you to revisit all your scenes and re-assign materials to objects. Another possible way to remove data links is in Material Properties by shift clicking the x next to fake user. I kind of like repairing each scene manually as I know the work is done and organized on the save and reload. But am curious if making changes via Blender File is a good technique.