AFP Sport looks at five moments that defined the German manager's time at Anfield:
2016: Dortmund delight
It took nearly four years for the trophies to start flowing for Klopp in England but there were memorable moments from his first season as Liverpool reached the Europa League final, where they lost to Sevilla.
Klopp faced a reunion with former club Borussia Dortmund in the quarter-finals.
After a 1-1 draw in the first leg, two early goals from the Germans at Anfield left Liverpool with a mountain to climb.
But the Reds roared back, with Dejan Lovren scoring a late winner as Klopp bounced up and down on the touchline, celebrating a 5-4 win on aggregate.
Liverpool would go on to reach four European finals under Klopp as he restored the English giants as a powerhouse in continental competition.
2019: Barcelona blown away
For all of Liverpool's rich history in European competition, arguably Anfield's greatest-ever night came in a remarkable fightback against Barcelona to reach the Champions League final in 2019.
A Lionel Messi-inspired Barca had won the first leg 3-0 at the Camp Nou.
Back at Anfield, they were demolished by an under-strength Liverpool, who were without two of their own talismanic front three in Mohamed Salah and Roberto Firmino.
In their absence, Divock Origi was the unlikely hero as he and Georginio Wijnaldum each scored twice in a stunning 4-0 victory.
2019: Champions League glory
After beating Barcelona, Tottenham were tamed as tens of thousands of Liverpool supporters turned Madrid red in celebration of a sixth Champions League title.
Salah and Origi scored the goals at the Metropolitano Stadium as Klopp finally got his hands on Europe's biggest prize after losing his two previous finals with Dortmund and Liverpool.
2020: First Premier League trophy for 30 years
Liverpool posted a then club-record 97 Premier League points in the 2018/19 season, but still missed out on the title by one point to a relentless Manchester City.
The following year they were not to be denied - even by the interruption to the season caused by the coronavirus pandemic.
Klopp's men won 26 and drew one of their opening 27 games on their way to racking up 99 points and claiming a first league title in 30 years.
The players had to lift the trophy at an empty Anfield because of Covid restrictions, but thousands of fans defied the ban on socialising to gather outside the stadium, setting off red flares.
2024: Unlikely final trophy
Klopp's goodbye did not reach a glorious crescendo as Liverpool's Premier League title challenge came off the rails in the final weeks of the campaign and they exited the FA Cup and Europa League.
However, there was still silverware to celebrate from his final season in the League Cup.
Virgil van Dijk's header minutes from the end of extra-time beat Chelsea 1-0 to secure an unlikely triumph for Klopp's under-strength side.
Liverpool were severely weakened by injuries and absences at the Africa Cup of Nations and Asian Cup when they arrived at Wembley.
But Klopp's faith in a clutch of teenagers paid off as they helped turn the tide in Liverpool's favour during extra-time before Van Dijk's stooping header broke the deadlock.