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Maricopa County seems like it would have to be one of the largest ones that also houses a major metro - 9,224 sq miles and per the census quick facts it had a population of 3,954,598 making it the 4th most populus county in the US behind LA County, Cook County and Harris County
Southern CA has 3 of the top 6 most populus counties
Even though, it isn't a "County" in the traditional sense, the Unorganized Borough in Alaska can be called the biggest. It is larger than France and Germany combined. It is also bigger than any other State besides Alaska.
Nassau has a density of 4,655 from the above census data
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