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Discover Ludwig"largest municipality" is correct and usable in written English.
You can use it to refer to the largest city or town in a particular area. For example, "The largest municipality in the state is the city of Seattle."
Exact(51)
At 54.7 square miles, Hillsborough is the largest municipality in Somerset County.
The city now has 10 million people and is the largest municipality in the world.
Black and Latino people are concentrated in the largest municipality, the city of York.
Shanghai is the largest municipality in China and one of the 10 largest in the world.
By 1970 it had a population of 570,000 – the fourth largest municipality in the country at the time.
Oklahoma City, the largest municipality in the state, lies at the centre of a six-county metropolitan area.
Similar(9)
Table 5 lists the ten largest municipality-industries by their output (in Colombian pesos) in 1997 in our sample.
The remaining four largest municipality-industry are "Coke, refined petroleum products and nuclear fuel" (Barrancabermeja), "Motor vehicles, trailers and semi-trailers" (Bogotá, D.C.), "Textiles" (Bogotá, D.C.) and "Rubber and plastics products" (Bogotá, D.C.).
The Delhi Municipal Corporation -- the world's second-largest municipality after Tokyo -- will test it soon.
With nearly 100,000 people in central New Jersey, Woodbridge is the state's sixth-largest municipality.
Waterbury, once a major brass manufacturing center, is Connecticut's fifth-largest municipality, with a population of about 107,000.
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Since I tried Ludwig back in 2017, I have been constantly using it in both editing and translation. Ever since, I suggest it to my translators at ProSciEditing.

Justyna Jupowicz-Kozak
CEO of Professional Science Editing for Scientists @ prosciediting.com