dumblonde recently answered a similar question.  She turned us all on to a sit about languages.
Here is a link from that site about Croatian.
http://www.ethnologue.com/show_language.asp?code=hrv
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Source(s):
http://www.ethnologue.com/show_language.asp?code=hrv

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Well technically Serbian, Croatian and Bosnian are almost same languages, mainly the dialects are different.

For the word "WHERE" Serbians say gdE. Croatians say gdIE. The meaning is same, the biggest difference is in the pronunciation.

But if you mean what is most similar to Croatian as in from a different country I would say it's Ukrainian, and then Russian.

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Croatian is a South Slavic language. The South Slavic languages have a large number of dialects and it is debatable which amount to a separate language. Politics enters into the debate as much as linguistics. They are all from the countries of the former Yugoslavia, except Bulgaria. I would suggest Bulgarian is the language that is the best answer to your question, as it is closely related but a clearly different language and country.
Source(s):
http://en.wikipedia.org/wiki/South_Slavic_languages

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