The deal is worth $29 million plus incentives, sources said.
The Pacers announced Carlisle's hiring on Thursday afternoon but did not disclose terms of his contract.
Carlisle spent 13 seasons in Dallas, becoming the franchise's winningest coach with a 555-478 record and leading the Mavs to the franchise's only championship in 2010-11. His resignation came a day after the franchise parted ways with longtime president of basketball operations Donnie Nelson, but Carlisle said the front-office changes in Dallas had nothing to do with his decision.
"You never want to get to a point where you ever feel like you're overstaying your welcome, and I just felt like this is the right time," Carlisle said Thursday. "I just have such great respect for [Mavs owner Mark Cuban] and everyone there, and I'm fortunate to move on to another great opportunity."
Cuban has said that he plans to hire a new head of basketball operations before finding Carlisle's replacement. Mavs legend Dirk Nowitzki has returned to the franchise as a special adviser to assist Cuban in those searches.
Sources told ESPN on Thursday evening that the Mavericks are finalizing a deal to make Hall of Fame point guard Jason Kidd the franchise's new head coach.
Cuban is also close to hiring longtime Nike executive Nico Harrison to a front-office leadership position, sources said. The Mavs are optimistic that vice president of basketball operations Michael Finley will remain with the franchise and work alongside Harrison, sources said.
Mavs assistant coach Jamahl Mosley, who has a particularly strong relationship with superstar guard Luka Doncic, was also expected to be among the coaching candidates considered in Dallas' search.
Carlisle on Thursday offered a strong endorsement of Kidd, whom Carlisle coached for four seasons in Dallas, highlighted by the Mavs' championship run.
"My hope is that Jason Kidd will be the next coach of the Mavs because he and Luka have so many things in common as players," Carlisle said. "I just think that it would be a great situation for Luka, and I think it would be an amazing situation for Jason. I'm the only person on the planet that's coached both of those guys and that knows about all of their special qualities as basketball players. To me, that just would be a great marriage, but that's just an opinion."
Carlisle previously coached the Pacers for four seasons (2003-04 to 2006-07), compiling a 181-147 record and making the playoffs three times, including an Eastern Conference finals appearance in 2003-04. He also was a top assistant under Larry Bird for three seasons (1997-98 to 1999-2000).
In his return to Indiana, Carlisle will replace Nate Bjorkgren, who was fired after one season as the Pacers' head coach. Indiana went 34-38 last season, when the team had several key injuries and Bjorkgren clashed with core players. The Pacers were eliminated in the play-in tournament, snapping the franchise's streak of five consecutive playoff appearances. Carlisle cited his trust in team owner Herb Simon as a reason the Indiana job was attractive to him.
"It's an exciting situation because there's upside here," said Carlisle, 61, who has a career record of 836-689, ranking 15th in career wins. "Getting back healthy is going to be a big part of that.
"[General manager Kevin Pritchard] and I have talked extensively about the roster. I like their roster. It's a team of skilled, unselfish guys that play hard. It's always possible that moves could be made before the season, but I think Kevin and I are both very excited about getting the roster healthy and seeing what this team can be."
In the statement announcing Carlisle's hiring, Pritchard said Carlisle is "a proven winner with a championship and will be a Hall of Fame coach.
"He has demonstrated throughout his career an ability to build something with sustainable success. He has great respect for our franchise and our fans from his previous times here. We are very happy to welcome him back to Indiana," Pritchard said.
The Mavs, meanwhile, have not advanced past the first round since winning the title a decade ago, having undergone a rebuilding process during that span. They were eliminated the past two seasons by the LA Clippers, losing in seven games this year after winning the first two games of the series on the road.
In the wake of the Mavs' elimination, Cuban told ESPN that he would not consider a coaching change this offseason.
"Unless you have someone you know is much, much, much better, the grass is rarely greener on the other side," Cuban said then.
However, sources said that simmering tension between Carlisle and Doncic, the 22-year-old two-time first-team All-NBA selection, had become a concern within the organization. Carlisle said he reached the conclusion that his departure from Dallas would be "mutually beneficial."
"I just sent [Doncic] a message thanking him for three amazing years," Carlisle said Thursday. "I learned many things from him, and I told him that I'm glad I'm only going to see him twice a year. I mean it in the most complimentary way, of course.
"I think he's the best young player in the world. I think these three years set up as a major springboard for the next 10 for him. I expect him to be an NBA champion. I expect him to be a multiple MVP winner. I just have an amazing level of respect for his abilities and his grasp of the game. He's truly a once-in-the-generation type player."
The Mavericks will not ask the Pacers for compensation despite Carlisle resigning with two years remaining on his contract, sources said. Cuban did not want to complicate Carlisle's search for a new coaching opportunity.
"He is a trusted friend and a basketball soulmate," Carlisle said of Cuban. "You occasionally come across people that change your life, and he changed my life, and he changed my family's lives. It's very difficult to come up with a simple statement to thank somebody for the 13 years that I've had with him.
"I just have an amazing amount of gratitude to the city of Dallas, the Mavericks organization, all the players and coaches that I've had an opportunity to work with. Dirk, J-Kidd, [Jason Terry], Luka, Tyson [Chandler], Shawn Marion, J.J. Barea -- there's just so many. It would be very emotional to just try to express all the feelings that I have about it."