The deal, which runs through the 2020 season, is the largest ever awarded to a player subject to American draft rules with less than two years of service time. Cubs first baseman Anthony Rizzo signed a $41 million, seven-year contract last May.
Simmons, 24, showed power potential in 2013, when he hit 17 home runs, but he earned the big contract with his defence. He won his first Gold Glove award in 2013, when he led the major leagues with 499 assists.
"We feel that Andrelton is one of the premier shortstops in the game today, and we are happy that we were able to agree on this multiyear contract," general manager Frank Wren said in a statement released by the team.
The Braves this month also reached multiyear agreements with first baseman Freddie Freeman, outfielder Jason Heyward, closer Craig Kimbrel and right-hander Julio Teheran, committing $280.7 million to the rising stars, including Simmons.
Simmons hit .248 and drove in 59 runs last season. He earned the new contract after playing in only 206 career games.
Simmons received a $1 million signing bonus and will earn $1 million this season. He will earn $3 million in 2015, $6 million in 2016, $8 million in 2017, $11 million in 2018, $13 million in 2019 and $15 million in 2020.
It has been a busy month for the Braves and Wren.
On Sunday, the team agreed to a $42 million, four-year contract with Kimbrel, 25, the All-Star closer. That came two days after the 23-year-old Teheran agreed to terms on a six-year, $32.4 million deal.
Earlier this month, the Braves announced multiyear deals with a pair of 24-year-old hitters — Freeman and Heyward.
Freeman, the All-Star first baseman, agreed to the biggest contract in Braves history — $135 million for eight years.
Of all the new deals, only Heyward's is for fewer than four years. Heyward, the outfielder who won his first Gold Glove in 2012, signed for two years and $13.3 million.
Even management has been included in the wave of new deals. Manager Fredi Gonzalez and Wren also have been given contract extensions.
Simmons ranks with Freeman, Kimbrel, Teheran, Heyward, Justin Upton, left-hander Mike Minor and others as the foundation for the Braves' future. Chipper Jones retired after the 2012 season, and Tim Hudson and catcher Brian McCann departed as free agents after last season, leaving the team that won 96 games last year with a young roster.
Simmons hit only .216 against left-handers last season, and he hit only .219 in 283 at-bats as a leadoff hitter. The team took off when Heyward was moved to the leadoff spot, and Simmons was more productive in other spots in the lineup.