Pujols hit No. 661 in the fifth inning to break the tie with Mays, then connected again in his next at-bat.
The 40-year-old Pujols now trails only Barry Bonds (762), Hank Aaron (755), Babe Ruth (714) and Alex Rodriguez (696).
The Angels quickly congratulated Pujols on Twitter.
Congratulations, Albert. What an incredible accomplishment 🙌 pic.twitter.com/dxQObF7tI8
— Los Angeles Angels (@Angels) September 19, 2020
Pujols had hit just four home runs this season before posting the 60th multi-HR game of his career and first since May 11 last year at Baltimore. He finished with three hits on the night.
After tying Mays’ mark last Sunday in Colorado, he passed the Hall of Famer with a solo drive to left. Pujols sent a 1-2 fastball from Wes Benjamin into the Rangers’ bullpen. Pujols pointed to the dugout and did a fist pump as he approached third base.
After the Rangers rallied to get within 3-2, Pujols led off the seventh with No. 662 off Demarcus Evans into the Angels’ bullpen to extend the lead.
Pujols has gone deep to left 330 times in his career and 362 have come with the bases empty.
Pujols, who has one more season left on his contract with the Angels after this year, has 108 home runs at Angel Stadium, which is only three behind the 111 he hit at new Busch Stadium, which opened in 2006.
Benjamin was the 427th different pitcher Pujols homered against in his career and Evans, making his MLB debut, became the 428th two innings later. Only Bonds has homered against more (449).
The Associated Press contributed to this report.