Word 2007 & later have a maximum file size of 512MB. Do bear in mind that Word 2007 & later do much more content compression for docx files than the older versions could with doc files, so you can't really compare one with the other. All Word versions also have a limit of 32MB on the unformatted text content. The file size limits for previous versions were not published.

Just opening & rendering a 512MB file will take a long time, so ask yourself whether your doing things the right way. Is there a good reason for not working with smaller files?

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Cheers,
Paul Edstein
[Fmr MS MVP - Word]