The first part of the settlement is the museum. I was worried the museum wouldn't hold the attention of young ones, but it surprisingly did. They liked the recreations of the Elizabethan English town, the dioramas depicting Powhatan and African villages as they looked before white settlers/slavers came to them. They especially were drawn to the full size recreations of a Native American hut, a slave quarters, and a traditional colonist's home that they could walk through. It helps that a lot of the museum's exhibits are touchable and interactive. They could pet the furs, open and shut the under the floor storage compartments, and sit by the flickering fires in the hearth.
(I was also worried that the museum would focus more on the plight of the colonists and not the Native and African populations that also were affected by colonization. But I shouldn't have. The presentation is one of the most balanced and honest I have seen and is presented in a way that honors each culture while showing how it was affected when it came in contact with the white settlers. I especially recommend stopping and watching the video interpreters talking about how their lives changed when the settlers came.
Outside the museum, we walked the short way to the recreated Powhatan town. There, the kids ran in and out of the dwellings and ground corn, played games, and talked to the re-enactors who were weaving baskets, gardening, and building canoes. Everyone was super knowledgeable there and inside the recreated fort itself, our next stop. Have you ever tried on armor? Or played ten-pins? Or looked over a 17th century doctors tools? You can at the fort.
Finally, our last (and probably most fun of all) stop was at the river, where we boarded replicas of the three ships that brought the English colonists to Jamestown. It was (as Anouk said) SO COOL. You're actually on a ship in the water, you can explore below decks, learn how to navigate by the stars and measure the speed of the boat, hold cannon shot and cannonballs, and tuck yourself into a teeny tiny sailors' berth.
If you are a Virginia resident, I recommend taking advantage of the annual pass if you're thinking of making a visit. The pass costs $23 per adult (over 13) and gets you unlimited access for a year to both Jamestown and the American Revolution Museum at Yorktown. (Historic Jamestown is a National Park site so admission is not included in the pass). It's only a few dollars more than the one-time day pass. And both sites hold pretty cool events on holidays and throughout the year. One is coming up this weekend at Jamestown -- a colonial trade fair -- and on July 4, Yorktown will host its Victory celebration.