I’ve only played the first so far. My best on my first playthrough (though it might’ve been supplanted by another; it definitely was overall by the top word in my next playthrough) was QUOTIDIANS (a word I only knew thanks to an MIT Mystery Hunt one year). Sadly, I cannot remember what my top on my second playthrough was, probably because it was much more common.
I just looked in the Hall of Fame and apparently it was NEUROSURGEON (12 letters). I can’t remember that game but it must have been a bitch to get. Apparently it doesn’t support Internet leaderboards anymore, which is too bad. Wikipedia says there’s a Bookworm Adventures out now, it looks really different.
Mine is CARBOHYDRATE. Just got it earlier today. Tried to add an “S” to it, but the game doesn’t allow 13-letter words. It just put an “X” through my last letter, and I had to settle for the singular.