Smith and Joe Johnson each scored 18 points, and the Hawks recovered in the fourth quarter to beat the Bulls 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.
Luol Deng had 20 points and eight rebounds, and Derrick Rose scored 19 points for the Bulls, who lost their third consecutive game.
The Bulls led 70-64 entering the fourth.
"We wasted, I thought, a pretty good effort," said Bulls coach Vinny Del Negro.
Del Negro said the Hawks "knocked us back on our heels a little bit" by opening the final quarter with an 8-0 run. Atlanta took the lead for good when a basket by Johnson with 7:46 broke a 72-all tie.
"They just caught on fire," said Rose. "We had them. They were just making some tough shots."