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If by "most valuable" you mean "largest denomination", the Series 1934 US $100,000 gold certificate is the highest-denomination bill ever printed by the US. These bills were specially printed to facilitate movement of large sums within the Federal Reserve System. They were never placed into general circulation. 42,000 were originally made; all but a few were recalled and destroyed when electronic funds transfers became possible.

The largest bills ever made for general circulation were $10,000 Federal Reserve Notes. They were last printed in 1945 although they carried the same 1934 series date as the $100,000 gold certificates.

Distribution of high-denomination bills ($500, $1000, $5000, and $10,000) was halted in 1969 by President Nixon in an effort to hamper their use in criminal transactions. The bills were never formally withdrawn from circulation but have essentially disappeared over the subsequent decades.

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Q: Is the most valuable piece of money ever printed in the US a 100000 bill?
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