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Ages back, I did - think GSC and then DPPt. Since then technically no because I just sent them to Bank pretty sure, and so they are sitting there for all time. :V
I did when i thought they were special, i liked the puzzle game in Gold/Silver/Crystal where you had to complete the puzzle to fall down and get to meet new unknown, at that time i thought something special would happen..
I collected all the Unown once in FireRed, and ended up transferring them all over to HeartGold just so I didn't have to do it again. I still actually have them on my file, and with the hassle of trying to move Pokemon from Gen 4 to 5, they'll probably just stay there forever, haha.