Your best option might be doing each move separately.

That’s because for this kind of move it most likely would not be considered an en-route pickup. Long distance moving companies like to combine shipments so that they have a full load; keeping a space empty on the truck all the way from NY to North Carolina would probably turn off some moving companies. 

That said, these are challenging times, so a moving company might be interested in doing the move as an enroute pickup even if it's out of the norm for them.  

Your best bet is probably contacting an agent for a van line company in your area and telling them your situation. A van line is just a large moving company that has agents all over the country (it’s analogous to how a franchisor works). Because van lines have an agent system, they’re probably best able to handle your situation.

They could either do your wife’s move as an enroute pickup, or they could work with their van line agent in North Carolina to give you a quote for a second move down there. Even if it’s done as two separate moves, they might give you a break on the price. Also, it’ll be easier for them to coordinate delivery of your items to Atlanta if you want to get them there at roughly the same time.

You should definitely have an in-home survey done so the movers know exactly what they’ll be moving at both locations. And you should try to get quotes from two separate van lines so you know what you’re looking at as far as costs.

Best of luck!