Well, isn't that just a happy little question! Two thirds of a gallon is like taking a big hug from nature - it's about 0.67 gallons. Just imagine all the beautiful paintings you could create with that much paint! Remember, there are no mistakes, just happy little accidents.
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A US gallon is 16 cups, so 1/3 of a gallon is 16/3 = 5 1/3 cups. 2/3 gallon is twice as much which is 10 2/3 cups.
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2/3s of what? gallon, pint, quart, liter?
666.66... recurring mL.