Just a couple of cautionary statements and maybe some help to find sources.
First of all if you use Ancestry please do not use their trees for sources. If you are using things from records that is ok but please don't use trees as they are often filled not only with errors but also with people who never existed. There are a lot of fraudulent genealogies written for the time period you are looking at and a number of these frauds were picked up by likely well meaning folks who then created ancestry trees and helped to perpetuate bad genealogy.
For pre-1700 time period in the US sources are notoriously sparse. Look for wills, land grants, indenture contracts, church records, and local histories. Also pre-1700 civil records may not exist in the US but in the country that governed that specific location in a given time period.
This is list of know frauds Make sure you don't use any of these as sources.
https://www.wikitree.com/wiki/Category:Fictitious_and_Legendary_Genealogy
On the positive side, this is a very hard but useful undertaking. Here are some sources that might assist you
https://www.wikitree.com/wiki/Category:Source and here are some pre-1500 that can also be used for pre-1700 annotated sources
https://www.wikitree.com/index.php?title=Space:Pre-1500_Resource_Page&public=1
And post questions about someone you are researching here in G2G because pre-1700 time period is a really good place to collaborate as the records are spotty at best.
Because a lot of these folks are likely tied to England this link to the records of Parliament up to 1707 may be of help
http://www.rps.ac.uk/ and
http://perqtax.homestead.com/files/perqpre1700.html
You may want to give a balanced perspective of Loyalist vs Revolutionary and remember these feelings began to forment long before the war in 1776 This book raises a different view than presented by George Chalmers an English historian with a decidedly negative view of colonists.
http://nc.lostsoulsgenealogy.com/books/notesoncolonialnc.pdf
There are good resources at some of the universities and colleges in their rare books rooms in the local area too.
Oh and one more thing, make sure to use the correct location names because North Carolina came into existence December 7, 1710 during a meeting of the Lords Proprietors held at Craven House in London. Evidently the term North Caroline was in use by 1712 as a result of this decision to split the former colony into North and South.
Prior to the English settlement of Roanoke in the latter 1500s, the Spanish claimed the area we call North Carolina. Make sure to check the naming conventions here:
https://docs.google.com/spreadsheets/d/1jlRaiRtaMEpsPdeuRLS2ids4HAXJyGVCKiQyEMh4NNE/edit#gid=667189750 and
https://www.wikitree.com/wiki/Space:North_American_Place_Names