Simic, who lives in Strafford, will replace another New Hampshire poet — Donald Hall of Wilmot.
Simic takes up his duties in the fall, opening the library's annual literary series Oct. 17 with a reading of his work. He also will be the featured speaker at the Library of Congress National Book Festival on Sept. 29 in the poetry pavilion on the National Mall.
Simic taught at the University of New Hampshire for 34 years before moving to emeritus status. He won the Pulitzer Prize in poetry in 1990 for his book of prose poems, "The World Doesn't End." He also is an essayist, translator, editor and professor emeritus of creative writing and literature.
The poet laureate promotes poetry across the nation.
In a statement from Washington, Librarian of Congress James Billington said Simic handles language with the skill of a master craftsman. He has written 18 books of poetry.
"The range of Charles Simic's imagination is evident in his stunning and unusual imagery," Billington said. "He handles language with the skill of a master craftsman, yet his poems are easily accessible, often meditative and surprising. He has given us a rich body of highly organized poetry with shades of darkness and flashes of ironic humor."
Born in Yugoslavia in 1938, Simic arrived in the United States in 1954. He has been a U.S. citizen for 36 years.
"I am especially touched and honored to be selected because I am an immigrant boy who didn't speak English until I was 15," he said.
Simic's childhood was disrupted by World War II. He moved to Paris with his mother when he was 15 and joined his father in New York a year later. They then moved to Oak Park, a suburb of Chicago.
Simic graduated from the same high school as Ernest Hemingway. He started writing poetry in high school to attract girls, he said.
He attended the University of Chicago, working nights in an office at the Chicago Sun-Times, but was drafted into the Army in 1961. He served two years.
He earned his bachelor's degree from New York University in 1966.
He wrote and translated poetry from 1966-1974. He also worked as an editorial assistant for a magazine.
He married fashion designer Helen Dubin in 1964. The couple has two children.