Despite finishing top of the newly formatted group stage with an impressive 21 points, Arne Slot's side faced a difficult last-16 draw against a formidable PSG, who remain unbeaten in Ligue 1 and, in Slot's words, are "statistically the best team in Europe."
Liverpool held a 1-0 aggregate lead after the first leg, but PSG's Ousmane Dembele levelled the tie in the return fixture.
The two sides could not be separated across 210 gruelling minutes, forcing the contest into penalties, where PSG triumphed 4-1 to seal their place in the quarter-finals.
Slot expressed pride in his team's performance but hinted that he may approach the league phase of next season's Champions League differently.
"I am feeling disappointed about being knocked out. I do feel in the end of the season, it does matter how we presented ourselves in Europe," Slot told the media after the game.
"I just said, we were not in the Champions League last season and this season we really showed ourselves. We can be proud of what we did. We won seven games in a row and then we played with our substitutes and lost against PSV.
"I think we played last week not our best game but today we saw a completely different Liverpool. We go out in a way that I think has impressed Europe.
"It is something now to take into consideration about how much worth it is to end up first in the league table if you can face Paris Saint-Germain in the next round.
"It is what it is. Maybe I am [speaking] too soon now but maybe it would be more fair that after the round in between, the one that wins the league table plays against the team that is lowest position after the teams have played.
"But that is also because we were so unlucky to play Paris Saint-Germain because we could have also gone to the other side of the draw.
"In the end, if you want to win the tournament you have to beat teams like Paris Saint-Germain and that's what we didn't do today after an incredible first 90 minutes of football from us."
Liverpool have made a mid-season change to their backroom staff after concerns over their defensive performance from dead-ball situations, confirming the departure of set-piece coach Aaron Briggs.
Paris Saint-Germain sporting director Luis Campos has said the club's owners are determined to extend Luis Enrique's contract, underlining how central the head coach is to their long-term plans.
Arne Slot hailed Florian Wirtz's performance as "special" after the midfielder scored his first goal for Liverpool in a 2-1 Premier League victory over Wolves at Anfield.
Liverpool and Arsenal both had to dig deep for victories on Saturday, while impressive Aston Villa powered to an eye-catching comeback win at Chelsea.
