Officers were called to the couple’s New Canaan home at about 20:00 local time on Saturday to investigate “a family dispute”.
Paul Simon and Edie Brickell, who have been married for more than 20 years, are due to appear in Norwalk Superior Court on Monday.
Paul Simon, 72, first found fame as one half of folk duo Simon and Garfunkel.
Edie Brickell, 48, was lead singer of Edie Brickell & New Bohemians.
The folk-rock band had a big hit with their debut single What I Am in 1988 and the track was covered by former Spice Girl Emma Bunton in 1999.
Earlier this year, Edie Brickell won a Grammy award with Steve Martin for best American roots song, Love Has Come For You.
Edie Brickell is due to start touring in May with Steve Martin and the Steep Canyon Rangers across the US and Canada.
A New Canaan police news conference is expected to take place later on Monday.
According to local media, Paul Simon and Edie Brickell have lived in New Canaan with their three children for years. New Canaan Police did not want to release their address.
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