As answered by others earlier, yes there likely needs to be a NC return filed. Assuming you file a joint federal return he has the option to file a separate NC return with only his income and deductions reported. Below is an extract from the NC Department of Revenue for reference. So if his gross income is below the NC filing threshold then a return is not required; but if you want the withholding refunded, you must file.
Additionally, TurboTax desktop products make this task easier. Here is a link that will help with the process. Basically, you will create and file your joint federal and NJ returns. You would then create a "Mock" federal separate return with only your spouse's income and deductions. This will flow to a NC separate return. You will need to print/mail the NC return because no federal separate return is being e-filed. Also per the extract below you include copies of both the separate and joint federal returns with your NC filing.
"If an individual chooses to file a separate North Carolina return, the individual must complete either a federal return as married filing separately, reporting only that individual's income and deductions, or a schedule showing the computation of that individual's separate income and deductions and attach it to the North Carolina return. In addition, a copy of the complete joint federal return must be included unless the federal return reflects a North Carolina address."
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