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Daniel Sturridge and James Milner gave the Reds the advantage before Thomas Meunier pulled one back and Kylian Mbappe appeared to have secured a draw. But Firmino fired home in the dying seconds to win the duel between German coaches Juergen Klopp and Thomas Tuchel, and put Liverpool top of Group C.
Red Star Belgrade drew 0-0 with Napoli in the other game while in Group A Atletico Madrid recovered to win 2-1 in Monaco and Borussia Dortmund won 1-0 at Club Brugge.
In Group D, 10-man Galatasaray defeated Lokomotiv Moscow 3-0 and Porto missed one penalty and scored another en route to a 1-1 draw at Schalke.
Earlier, Argentine star Lionel Messi struck three times in one of the Group B early kick-offs as Barcelona crushed PSV Eindhoven 4-0 while Inter Milan shocked Tottenham Hotspur 2-1.
Holders Real Madrid begin their campaign at home to Roma on Wednesday.
Beaten finalists last season, Liverpool started quickly in attacking their vociferous fans at the Kop end of Anfield but PSG looked to have weathered the early storm.
"It was really important we started like we did," Klopp told BT Sport. "We were so strong and good with the ball.
"We needed all of our focus and we covered a lot of yards and closed all of the gaps."
PSG fell behind on 30 minutes when Sturridge, starting as Firmino only made the bench with an eye injury, headed in Andy Robertson's cross.
Juan Bernat fouled Georginio Wijnaldum to give Milner the chance to net from the spot but Meunier cut the deficit before half time.
PSG's stars of Neymar and Mbappe were starved of service and Liverpool were denied a third when Mohamed Salah's goal was disallowed for a foul on goalkeeper Alphonse Areola.
Salah's misfortune continued as his misplaced pass set up Neymar to drive into the box and Mbappe levelled from his pass.
But Liverpool, who had dominated the second period, were not to be denied and Firmino created space in the box to shoot across Areola into the bottom corner for the winner.
"We followed our instructions and tried to cause them problems on the break," PSG midfielder Adrien Rabot said. "We scored two goals and it wasn’t enough, but there were lots of positives.”
Red Star, champions in 1991, were making their debut in the modern version of the competition and fought bravely to hold Napoli to a draw in the other Group C match.
In Barcelona, Messi struck either side of Ousmane Dembele's wonderful solo goal to end the resistance of PSV in the Camp Nou and Samuel Umtiti's red card did little to spoil the mood of the hosts.
"Messi's free-kick goal was absolutely majestic," Barca coach Ernesto Valverde said of the set piece 32nd minute opener. "It's not that we get tired of saying such things about him – I'd like to keep saying that forever."
Dembele cut beyond his man to shoot home from the edge of the box to make the points safe in 75 and Messi's first time finish immediately made it three.
Umtiti picked up a second yellow for a thumping foul on Hirving Lozano but the Argentine star completed his eighth Champions League hat-trick two minutes from time.
Spurs were heading for victory thanks to Christian Eriksen's second half deflection but a brilliant volley from Mauro Icardi (85) and Matias Vecino's close-range header in injury time turned the tie.
"Obviously it was a team effort and the victory is what counts the most," Inter defender Stefan de Vrij told UEFA. "Many of us were playing in the Champions League for the first time but it's difficult to ask for a better debut."
Monaco led Atletico thanks to Grandsir capitalizing on bad defending but Diego Costa and Jose Gimenez gave the Madrid side a winning start en route to a potential final in their own stadium next year.
In Brugge, Borussia Dortmund grabbed a winner through birthday-boy Christian Pulisic five minutes from time.
Group D is led by Galatasaray as Garry Rodrigues, Eren Derdiyok and Selcuk Inan, from the spot, downed Lokomotiv despite Badou Ndiaye seeing two yellow cards.
The spoils were saved elsewhere as Schalke's Ralf Faehrmann saved an early penalty from Alex Telles but was beaten from the spot by Otavio to cancel out Breel Embolo's opener.
Red Star Belgrade drew 0-0 with Napoli in the other game while in Group A Atletico Madrid recovered to win 2-1 in Monaco and Borussia Dortmund won 1-0 at Club Brugge.
In Group D, 10-man Galatasaray defeated Lokomotiv Moscow 3-0 and Porto missed one penalty and scored another en route to a 1-1 draw at Schalke.
Earlier, Argentine star Lionel Messi struck three times in one of the Group B early kick-offs as Barcelona crushed PSV Eindhoven 4-0 while Inter Milan shocked Tottenham Hotspur 2-1.
Holders Real Madrid begin their campaign at home to Roma on Wednesday.
Beaten finalists last season, Liverpool started quickly in attacking their vociferous fans at the Kop end of Anfield but PSG looked to have weathered the early storm.
"It was really important we started like we did," Klopp told BT Sport. "We were so strong and good with the ball.
"We needed all of our focus and we covered a lot of yards and closed all of the gaps."
PSG fell behind on 30 minutes when Sturridge, starting as Firmino only made the bench with an eye injury, headed in Andy Robertson's cross.
Juan Bernat fouled Georginio Wijnaldum to give Milner the chance to net from the spot but Meunier cut the deficit before half time.
PSG's stars of Neymar and Mbappe were starved of service and Liverpool were denied a third when Mohamed Salah's goal was disallowed for a foul on goalkeeper Alphonse Areola.
Salah's misfortune continued as his misplaced pass set up Neymar to drive into the box and Mbappe levelled from his pass.
But Liverpool, who had dominated the second period, were not to be denied and Firmino created space in the box to shoot across Areola into the bottom corner for the winner.
"We followed our instructions and tried to cause them problems on the break," PSG midfielder Adrien Rabot said. "We scored two goals and it wasn’t enough, but there were lots of positives.”
Red Star, champions in 1991, were making their debut in the modern version of the competition and fought bravely to hold Napoli to a draw in the other Group C match.
In Barcelona, Messi struck either side of Ousmane Dembele's wonderful solo goal to end the resistance of PSV in the Camp Nou and Samuel Umtiti's red card did little to spoil the mood of the hosts.
"Messi's free-kick goal was absolutely majestic," Barca coach Ernesto Valverde said of the set piece 32nd minute opener. "It's not that we get tired of saying such things about him – I'd like to keep saying that forever."
Dembele cut beyond his man to shoot home from the edge of the box to make the points safe in 75 and Messi's first time finish immediately made it three.
Umtiti picked up a second yellow for a thumping foul on Hirving Lozano but the Argentine star completed his eighth Champions League hat-trick two minutes from time.
Spurs were heading for victory thanks to Christian Eriksen's second half deflection but a brilliant volley from Mauro Icardi (85) and Matias Vecino's close-range header in injury time turned the tie.
"Obviously it was a team effort and the victory is what counts the most," Inter defender Stefan de Vrij told UEFA. "Many of us were playing in the Champions League for the first time but it's difficult to ask for a better debut."
Monaco led Atletico thanks to Grandsir capitalizing on bad defending but Diego Costa and Jose Gimenez gave the Madrid side a winning start en route to a potential final in their own stadium next year.
In Brugge, Borussia Dortmund grabbed a winner through birthday-boy Christian Pulisic five minutes from time.
Group D is led by Galatasaray as Garry Rodrigues, Eren Derdiyok and Selcuk Inan, from the spot, downed Lokomotiv despite Badou Ndiaye seeing two yellow cards.
The spoils were saved elsewhere as Schalke's Ralf Faehrmann saved an early penalty from Alex Telles but was beaten from the spot by Otavio to cancel out Breel Embolo's opener.
