Not sure if this passes for a "natural" remedy, but it's the first thing that I've known to help my particular RLS, so passing it on. Potassium Gluconate. It's sold in the vitamin/mineral section of the department or drug store, usually in 595 mg doses. I take one capsule before bed and it improves my condition. This would suggest that in my case a potassium deficiency might pertain to the RLS. Natural foods high in potassium include sweet potatoes and bananas. I also make certain not to go to bed cold (I find it advisable to keep warm, at least to start the night).