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Some candidates, although identifying the single largest secret will be hard:
WWII code-breaking secrets: Ultra is the most famous, but the Magic secrets were also very important. Perhaps a hundred people knew all about Ultra, but thousands knew that they were working on code-breaking and kept that quiet for decades after the end of the war.
The location of the invasion of north-west Europe in 1944. This was so important that a large deception project, Operation Bodyguard was set up to conceal it. The secret was not kept for a long time, but a large number of people knew it in the weeks before the invasion.
The idea of "staged radiation implosion", also known as the Ulam-Teller design for a hydrogen bomb. This was invented in the US in the early 1950s, and kept secret until 1979, although several countries re-invented it.