It was just the Dutchman's fourth defeat since taking over at the Anfield helm, after one loss in each of their respective Premier League, Champions League and Carabao Cup campaigns.
There were 10 changes from the side that booked Liverpool a place in the Carabao Cup final with the 4-0 second-leg win over Tottenham Hotspur.
However, the wholesale alterations failed to live up to expectations and as a consequence, the Reds endured a difficult afternoon on the south west coast.
Speaking during ITV's coverage of Exeter and Nottingham Forest, Keane claimed that the switch from Slot backfired and there will be lessons learned at the club.
"It's up there with the biggest I think really," he said. "When you see how well Liverpool are going, absolutely brilliant, scoring lots of goals, they made lots of changes which you thought the manager might do and he's taken a gamble. It's backfired on him.
"Credit to Plymouth who have been having a difficult season, in terms of giving goals and their home record which is not great. So that is definitely one of the biggest shocks out there.
"Lessons to be learned, particularly for the young players at Liverpool. It's real football whatever you're coming through, reserves, academy football. That was proper football and Plymouth really wanted it.
"When you're the underdog and you get the first goal, you have something to hold onto and to keep a clean sheet, [it's a] great effort by Plymouth."
Ian Wright added: "In the end, they [Plymouth] deserved it and I think it says a lot about the players on the fringe of Liverpool because you could see in the interviews that Arne Slot was having. Roy did you see him?
"He wasn't happy. He found out a lot about a few of those on that day."
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