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Admittedly it's an unusual definition of great, but my favorite is former White Sox catcher Moe Berg. Basically, imagine if Yadier Molina was a lawyer, and in his retirement from baseball, a spy:
"His best year was 1929, when his batting average (.288) and RBIs (47) were career highs. That season he caught 106 games for the Chicago White Sox and allowed only five stolen bases. Besides a strong arm, Berg had fast reactions and shrewd judgment. The best White Sox pitchers, Ted Lyons and Tommy Thomas, always requested Berg as their batterymate. 'In the years he was to catch me, I never waved off a sign,' said Lyons, a Hall of Fame righthander.
"When World War II began, Berg was first a U.S. goodwill ambassador in Latin America and then a spy in Europe, where, as Remus, he met Flute. They seemed an unlikely pair, but perhaps they really weren't. For Moe Berg could get along with anyone, if only for a time. 'Marvelous!' he would say, adjusting his fedora. 'Wonderful!' And then one of the most extraordinary characters in baseball or any other profession would vanish."
Nicholas Dawidoff's 1992 cover story on Moe Berg is one of the best things Sports Illustrated has ever published. The Vault, incidentally, is like if someone took most of my happy reading memories from childhood and put them all in one place for free.