The best playing-cards were so called because the wrapper, or “duty card” (when cards were subject to excise duty) contained the portrait of the Great Mogul. Those cards which contained some mark, speck, or other imperfection, were called “Harrys.”
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Entry taken from Dictionary of Phrase and Fable, edited by the Rev. E. Cobham Brewer, LL.D. and revised in 1895.