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I mean after scalding and covering in weed cloth. If it can survive all that it's time to bring out the flame thrower! :)

A non-toxic way to kill weeds/unwanted plants is boiling water. I have found it more effective than some of the vingegar & soap homemade weedkiller recipes out there, if you want to avoid Round-Up. Hopefully the tree roots would survive if the lilies-of-the-valley don't totally surround the tree...

I agree, it looks like Lily of the Valley. Does it have a nice smell? If it does I would be pretty sure that's what it is. It looks naturalized, so may be hard to fully remove, but it's poisonous enough I would fence off whatever you can't remove. All parts are poisonous, leaves, flowers and...