Should I select exempt from withholding on VA-4? I live in VA and work in NC. The company continues to withhold taxes from both states. I have completed form VA-4B.

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No, you should not file form VA-4 because there is not a reciprocal agreement in place between VA and NC. Your income will be subject to tax in both states and you will be eligible to claim a credit for taxes paid to another state on your VA tax return. Completing form VA-4B is appropriate and all you need to do.