The person spoke on condition of anonymity because the deal had not been announced.
Pujols' contract is only the third in baseball to break the $200 million barrier, following Alex Rodriguez's $252 million, 10-year deal with Texas before the 2001 season and A-Rod's $275 million, 10-year contract with the Yankees before the 2008 season.
In addition, the Angels agreed to a five-year contract with left-hander C.J. Wilson, a deal worth about $75 million, a person familiar with that deal said, also on condition of anonymity because it had not been announced.
Pujols has spent all 11 of his major league seasons with the St. Louis Cardinals, becoming a franchise icon second only to Stan Musial. St. Louis also offered him a 10-year deal, but he chose to leave the Gateway City for sunny California.
"He left a pretty good impact over there, I don't think fans will soon forget what his contributions were," said former Cardinals manager and star Joe Torre, now an executive with Major League Baseball. "I still think the St. Louis fans are going to be more appreciative than angry."
The Angels made the move as the financially troubled Los Angeles Dodgers are in the process of being sold by Frank McCourt in U.S. Bankruptcy Court, a move that could give the region's NL team a new wealthy owner next year. The Dodgers could aggressively bid for talent a year from now, giving them a boost in the regional competition for fans' attention.
Pujols led the Cardinals to a World Series title this fall -- his second with the team in the last six seasons. He also had been pursued by the Miami Marlins, but they dropped out Wednesday after agreeing to a deal with left-hander Mark Buehrle that raised their free agent-spending to $191 million for three players.
The Cardinals exercised a $16 million option on Pujols' contract after last season. The slugger rejected a multiyear extension last offseason that was said to include a small percentage of the franchise and cut off negotiations on the first day of spring training.
Pujols' numbers in nearly every major offensive category are on a three-year decline, but he remains among the game's elite players. He hit 37 home runs last season, running his 30-homer streak to 11 years, and batted .299 with 99 RBIs. He led the Cardinals' improbable late-season surge and became only the third player to hit three home runs in a World Series game.
Yahoo Sports first reported the Pujols deal.
"For 2012, two wilds cards and no Albert Pujols. I'm happy," said Sandy Alderson, general manager of the Cardinals' NL rival New York Mets.