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Just head to the Steam Community page of the game you want to do it and find 'Browse' on the top, then 'Subscribed items', you will then see the 'Unsubscribe From All' button
You can also create a workshop collection in the same place for your old mods so you don't lost track on them as well, although the interface is not exactly friendly to select and might be slightly, I mean, utterly painful if you had a lots of mods
Just to be noted that if the mod maker removed the mod, you will not be able to download from Steam since you can't subscribe again, obviously xD