It is The Hermitage Museum in Saint-Petersburg, Russia. In terms of floor space and exhibits in a single building. Other current museums, in terms of the size of the building only, are nowhere near it.
However; the Smithsonian is the largest museum "complex" in the world AND has the largest holding of ANY museum in the world. When speaking of the size of a museum the number of exhibits is the most widely accepted parameter. By this measure the Smithsonian is indeed the largest museum in the world; nothing else comes close. Comprising 19 museums and 9 research facilities. It has over 136 million holdings of art, specimens, exhibits, etc. The Hermitage has "only" 3 million holdings but is has the largest collection of paintings in the world. The Smithsonian has 1.5 million books in it's library alone.
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American Museum of Natural History
smithsonian
The Smithsonian, Washington, DC is the world's largest museum complex and research organization composed of 16 museums and the National Zoo.
the Smithsonian
It had an extensive library the largest in the ancient world and people wanted to go to Alexandria's museum.