Swiss police said the robbery happened at the Emil Buehrle Collection on Sunday. The three thieves are at large.
The gang threatened a security guard before seizing the works. The art theft is one of the biggest in the world in the last 20 years.
It comes just days after two Picasso paintings were stolen near Zurich.
'Impossible to sell'
The four paintings stolen on Sunday are: Poppies near Vetheuil, by Claude Monet (1879), Count Lepic and his Daughters, by Edgar Degas (1871), Chestnut in Bloom, by Vincent Van Gogh (1890) and Boy in a Red Jacket, by Paul Cezanne (1888), police said.
A police statement said the three masked men entered the museum in central Zurich at about 1630 local time (1530 GMT).
One of the men threatened staff with a pistol, while the other two collected the paintings, it said.
They were then loaded into a white vehicle parked outside the museum, the statement said.
Police said one of the thieves spoke German with a Slavic accent, and described the robbery as spectacular.
"We're talking about the biggest ever robbery carried out in Switzerland, even Europe," Zurich police spokesman Mario Cortesi told journalists.
Museum director Lukas Gloor said the stolen paintings were "the four finest in the museum's collection", the AFP news agency reported.
Mr Gloor said the works were so well-known that it would be impossible to try and sell them on the open market.
The famous Emil Buehrle Collection contains some of the world's most important impressionist works, the BBC's Imogen Foulkes in Switzerland says.
Picasso's oil paintings - Head of Horse and Glass and Pitcher - were taken from an exhibition in the town of Pfaeffikon last Wednesday.
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The gang threatened a security guard before seizing the works. The art theft is one of the biggest in the world in the last 20 years.
It comes just days after two Picasso paintings were stolen near Zurich.
'Impossible to sell'
The four paintings stolen on Sunday are: Poppies near Vetheuil, by Claude Monet (1879), Count Lepic and his Daughters, by Edgar Degas (1871), Chestnut in Bloom, by Vincent Van Gogh (1890) and Boy in a Red Jacket, by Paul Cezanne (1888), police said.
A police statement said the three masked men entered the museum in central Zurich at about 1630 local time (1530 GMT).
One of the men threatened staff with a pistol, while the other two collected the paintings, it said.
They were then loaded into a white vehicle parked outside the museum, the statement said.
Police said one of the thieves spoke German with a Slavic accent, and described the robbery as spectacular.
"We're talking about the biggest ever robbery carried out in Switzerland, even Europe," Zurich police spokesman Mario Cortesi told journalists.
Museum director Lukas Gloor said the stolen paintings were "the four finest in the museum's collection", the AFP news agency reported.
Mr Gloor said the works were so well-known that it would be impossible to try and sell them on the open market.
The famous Emil Buehrle Collection contains some of the world's most important impressionist works, the BBC's Imogen Foulkes in Switzerland says.
Picasso's oil paintings - Head of Horse and Glass and Pitcher - were taken from an exhibition in the town of Pfaeffikon last Wednesday.
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Gang robs Zurich of top paintings
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