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I wanted to talk about the cities where the population is high. My correspondent told me we must say:

The most populace cities

Instead of:

The most populated cities

I don't understand how the noun populace can be used as an adjective. Can you explain that to me?

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You've misheard, but it's an easy mistake to make. What the person suggested was:

The most populous cities

Populace and populous are homophones—Oxford Dictionaries lists both as /'pɒpjʊləs/. Here are the definitions of the two words (from Oxford Dictionaries):

populace
NOUN

[treated as singular or plural] The people living in a particular country or area.
"the party misjudged the mood of the populace"


populous
ADJECTIVE

Having a large population; densely populated.
"the populous city of Shanghai"

As for why populous must be used instead of populated, it depends on the meaning you're trying to put across. If you wanted it to mean "cities with the most people," you'd be fine (in my opinion) using populated. If you wanted it to mean "cities with the highest population density," I think you'd have to use populous instead.

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    Populated just means "having people", at all. Calico, California, is not populated. If you wanted to say "cities with the most people," you'd need "most heavily populated" (and even that suggests density rather than absolute numbers). Jul 11 '17 at 14:51
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    This is also an extremely common mistake made by native writers. Jul 11 '17 at 17:12
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    Yeah ... it's possible that the OP didn't mishear, but the correspondent made a spelling mistake.
    – LarsH
    Jul 11 '17 at 19:18
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    @chrylis: Is it? Never seen it. Jul 12 '17 at 0:52
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    @LukeSawczak: I see people writing "populous" when they meant "populace" All. The. [insert expletive here]. Time. The reverse mistake is much rarer.
    – Martha
    Jul 12 '17 at 1:27

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