The three-time NL MVP and the fresh-faced catcher just three years into his major league career helped Los Angeles beat the Arizona Diamondbacks 3-2 on Thursday night.
"That was special," Smith said. "I'll remember being on base when he hit his first one as a Dodger and high-fiving when he touched home plate. I look at him as a teammate now, not really an idol."
Pujols sent an 0-1 pitch from Merrill Kelly to right field, with Josh Reddick jumping to the top of the wall in an attempt to make the catch. Smith, who singled leading off, scored. Pujols was greeted by high-fives from his teammates in the dugout.
The win gave the Dodgers a four-game sweep, outscoring Arizona 19-6. They went 8-1 on the homestand and have won four in a row and eight of nine.
Pujols joined the Dodgers from the Los Angeles Angels on a one-year deal Monday. His arrival has coincided with the Dodgers' winning streak, but he claims no credit.
"These guys are a heck of a ballclub," he said. "Before I got there, this team is probably the best team in the major leagues. They know how to win. It's great to be here. I feel like home."
At 41 years, 124 days, Pujols is the oldest Dodgers player with a home run since Rickey Henderson homered for them at age 44 in 2003, according to ESPN Stats & Information research.
The hit was his 3,256th, breaking a tie with Eddie Murray for 13th on the all-time list.
"It felt great just to give our team an early lead right there in the bottom of the second. It's always great," Pujols said. "Thank god for giving me the opportunity to hit the ball the other way, hit it out of the ballpark and give an early lead to our ball club."
The Associated Press contributed to this report.