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Hertz does, although I haven't tried myself. You can check Hertz's Armenian website (in English), where you'll also get the price and be able to book this exact service. Hertz's Terms and Conditions even has a special section on renting in One Direction specifically for Georgia.
From my experience I will like to advise you NANIKO car rental in Armenia. You can rent a car in Yerevan and leave it in Tbilisi. Also as I compared early (5 month ago) NANIKO was cheapest, so highly recommended.
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