Well, all my Catskill hikes have been outstanding but there have only been two of them! Overlook was, agreed, very cool with the tower and the old hotel foundations. We were up there at night with patches of fog which gave it a really great "creepy" factor. The other was a gorgeous traverse of
Twin and Sugarloaf that was loopable with a bicycle spot.
Mountain biking in the 'Gunks is great, too.