McCann's book was chosen from 10 shortlisted titles to win the world's most lucrative literary prize worth 100,000 euro (?88,000).
Judges praised the author's story of colliding cultures set in 1970s New York as a "remarkable literary work".
It beat 161 other titles nominated by 166 libraries worldwide.
McCann is the second Irish author to win the prize after Colm Toibin's success in 2006 for The Master.
Let The Great World Spin was the most popular choice of libraries worldwide, receiving 14 nominations from libraries in countries including Ireland, Germany, Greece, Norway, the US and Canada.
The novel explores the intertwining lives of a radical Irish monk in the Bronx, an Upper East Side bereaved housewife, a proud young woman suffering years of hardship, a drug-addled young artist and a prostitute and her daughter.
The judges described the book as "a genuinely 21st century novel that speaks to its time but is not enslaved by it".
"Its beguiling nature leaves the reader with as much uncertainty as we feel throughout our lives, but therein lies the power of fiction and of this book in particular," they said.
The prize is open to novels published in the preceding year, written in any language by authors of any nationality, provided the book has been published in, or translated into, English.
Other finalists included Michael Crummey's Galore, The Lacuna by Barbara Kingsolver, The Vagrants by Yiyun Li and David Malouf's Ransom.
Also shortlisted were Little Bird of Heaven by Joyce Carol Oates, Jasper Jones by Craig Silvey, Colm Toibin's Brooklyn, Love and Summer by William Trevor and Evie Wyld's After the Fire, a Still, Small Voice.
Previous winners include last year's recipient, Gerbrand Bakker, for The Twin and 2009's winner Man Gone Down by Michael Thomas.
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