We visited a few years ago, before the Molokai Ranch closed down. Did a a hike (with a tour to avoid stink eye from the locals) at Halawa Valley to the falls. A great hike and very enjoyable. We arranged this through the Hotel Molokai.
I did the mule ride, and my husband hiked, to Kaluapapa. It was a great experience with lots of history. Note that the hike can be brutal on the way back up if you are not an experienced hiker.
Molokai is the most laid back island. Definately not a tourist destination, but still worth going for us. We found the locals to be the friendliest of all the islands we have visited. Everywhere we went they asked us where were from, where we were staying and what we liked to do, and then we were given suggestions of how to get the most out of our stay.
We planned to rent a 4X4 car while we were there. We went to pick it up only to find the car had not made the ferry and would not be arriving until the next day-which was fine we had no firm plans. But we spent an hour and a half just visiting with the woman who ran the company from a living room. We left with a map of the island with all the spots to stop on our travel along the island: ie: stop here for drinks and sandwiches nothing available beyond this point. Stop here for the best snorkeling on the island, etc.
We probably won't visit again, but we did enjoy our stay here quite a bit.