Smith and Joe Johnson each scored 18 points, and the Hawks recovered in the fourth quarter to beat the Bulls 91-81 on Friday night.
Smith also had 14 rebounds and 10 assists for his second career triple-double as the Hawks regrouped after trailing by six to open the final period.
He already had a double-double in points and rebounds when his offensive rebound and pass set up a 3-pointer by Mike Bibby with 2:13 remaining for his 10th assist, matching his career high. Bibby's basket gave the Hawks an 86-78 lead, matching their biggest advantage since the second quarter.
"It was big," Smith said. "It feels even better that we got the win."
Smith averages 15 points and 8.4 rebounds. He ranks third in the NBA with 2.19 blocked shots per game but needed help from Jamal Crawford, Johnson, Bibby and Atlanta's other perimeter shooters to reach 10 assists.
"I was passing it out and they were able to knock them down," Smith said.
Crawford had 17 points and Al Horford had 15.
Johnson said Smith "knows how to get in the paint, kick it out and make it easy for the other guys."
"He was unbelievable," Johnson said. "He was flying around. He had a total all-around effort tonight."
Hawks coach Mike Woodson said Smith was "phenomenal" and should have joined Johnson and Horford as Eastern Conference All-Stars.
"Josh has probably been our MVP," Woodson said. "I just wish he would've made that All-Star team because he has played like an All-Star this year for us. Everything that we have done from a team standpoint in terms of winning and losing has a great deal to do with the way he has played on both ends of the floor."
The Hawks had two 8-0 runs and outscored the Bulls 27-11 in the fourth.
The Bulls led 70-64 entering the fourth.
"We wasted, I thought, a pretty good effort," said Bulls coach Vinny Del Negro.
"Too many [Hawks] rebounds. Too many second shots. We hung in there. But in the fourth quarter they showed why they're one of the better teams."
Del Negro said the Hawks "knocked us back on our heels a little bit" by opening the final quarter with an 8-0 run, capped by Horford's jam.
Atlanta took the lead for good when a basket by Johnson with 7:46 broke a 72-all tie and started another 8-0 run for the Hawks.
"They just caught on fire," said Rose. "We had them. They were just making some tough shots."
The Hawks crushed the Bulls 118-83 on Dec. 9 in Atlanta in Chicago's most lopsided loss of the season, but the rematch was no runaway.
Atlanta ended the Bulls' recent trend of road wins against teams with winning records. Chicago closed a seven-game road trip from Jan. 18-29 with five consecutive victories over teams with winning records.
The Hawks improved to 21-5 at Philips Arena with their fifth straight home win.
Chicago's Kirk Hinrich had 13 points and a season-high nine rebounds.
Bulls center Joakim Noah was in Chicago receiving treatment for plantar fasciiitis, a painful irritation and swelling of the bottom of the heel. He is not expected to return to action until after the All-Star break. Brad Miller was the fill-in starter and had 10 points, all in the first half.
The Hawks scored the first eight points and led throughout the first half. Atlanta's biggest lead was 38-27 following a 3-pointer by Crawford.
The Bulls trailed only 50-46 at halftime and took their first lead at 56-55 on a Taj Gibson jam in the third quarter.
The Hawks' last triple-double was by Johnson against Oklahoma City on Dec. 23, 2008. Smith's first career triple-double came with 22 points, 12 rebounds and 10 assists on Jan. 23, 2008 at Denver.
The Hawks pushed back their Friday night planned flight for Saturday's game against the Wizards due to snow in Washington. The revised plan was for the team to fly Saturday morning. ... Atlanta's American Idol star "General" Larry Platt performed his original song "Pants on the Ground" during a timeout. ... Bulls F Chris Richard signed a 10-day contract and was in uniform but did not play.
LeBron James reacts to the Cavs setting the NBA record for threes made in a game, but believes the Cavs have work to do, saying, "We've got to be better in Game 3."
The Cavaliers drain 18 3-pointers in the first half and 25 for the game, a first half NBA record, a postseason-game record and a NBA record for threes in a game, in their rout of the Hawks.
The Rockets have interviewed veteran head coach Mike D'Antoni for their vacant position, while interim coach J.B. Bickerstaff has withdrawn his name from contention, according to sources.