As you can see, for reasons I don't think need explaining, most countries in the list are English-speaking or Spanish-speaking. However, there are some other notable contenders too:
Brazil - relatively few speak anything other than Portuguese.
Russia - relatively few speak anything other than Russian.
Japan/South Korea - although most learn English at school, they are only really taught to read and write it, not to speak it. Meanwhile, knowledge of other foreign languages is negligible.
North Korea - relatively few speak anything other than Korean.
Some countries I originally considered including but did not in the end:
China - Mandarin itself is an immensely difficult language to master; in any event, many Chinese speak it in addition to their regional languages.
France - the French nowadays are much better linguists than the stereotype, with around two-fifths able to speak English and lower, but still significant percentages who can speak German, Spanish and/or Italian.
Italy - the percentage who can speak foreign languages is not quite as low as in either Spain or the British Isles, even if it is still one of the weaker countries in Europe in that respect.
Puerto Rico - truly bilingual between Spanish and English.
Guatemala/Bolivia/Paraguay - at least half the population speak an indigenous language in addition to Spanish.
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