Without a doubt one of the most talented players in Liverpool's history. Mølby fought a hard battle with his weight, but his vision, immense skill, sublime passing and shooting ability more than made up for his lack of mobility. When Souness left Liverpool, Mølby was invited for a ten-day trial at Anfield. In his first match, against Home Farm in Ireland he took the ball on his chest, kneed the ball over the defender's head and volleyed it into the net. Joe Fagan signed him two days later. The great Dane had honed his trade at Ajax in Amsterdam for two and a half years prior to joining the European champions. He was in for a shock when he moved to Merseyside. "When we arrived at Carrow Road for my first game, we filed into the away dressing room," Mølby remembers. "I asked Ronnie Moran, ‘What do we do now?’ ‘Just get changed,' growled Ronnie. ‘Get yourself ready for the game, son.’ ‘What time do we go out to warm up?’ I asked. ‘You don’t have time to warm up, save your energy.’ I couldn’t believe what I was hearing. At Ajax, we spent about 25 minutes warming up." Despite the lack of preparation Liverpool got the right results.
Mølby was a regular in his first season as a defensive midfielder until he had to make way for Kevin MacDonald halfway through the campaign. Mølby was undoubtedly Liverpool's best player in the double 1985/86 season as Dalglish had great belief in him. "I couldn't believe such a creative player was languishing in Liverpool reserves and I couldn't wait to use him," Dalglish later said. "Jan had unbelievable feet and I defied anybody to state categorically which was the stronger, because either foot could propel the ball at unbelievable speed towards goal." Mølby enjoyed his freedom under Dalglish, playing sweeper on occasion as well as shadow striker behind Rushie. He scored 21 goals in 58 matches and delivered a man-of-the-match performance in the 3-1 win over Everton in the FA Cup final. Mølby's most famous goal came in the fourth round of the League Cup on 26 November 1985. Paul McGrath had put United 1-0 up but with roughly half an hour to go the Dane took charge at Anfield. "I took the ball off Norman Whiteside inside our own half. I went on a run past three or four United players and then shot with my right foot from about 20 yards. Gary Bailey, the United 'keeper, still insists it was the hardest shot he had ever faced. It's true that from the moment it left my boot to the moment it hit the net Gary didn't see it." A minute later Mølby added another from the penalty spot adding to his legend as the most prolific penalty-taker in Liverpool's history, scoring 42 out of 45 penalties. The secret to his spot-kick success was fairly simple: "If the goalkeeper didn’t move before I struck my shot I would always put it low to his right but if he moved I would go the other way. I guess that’s not something you can teach somebody it’s just something in their make-up."
Mølby started the following season well enough, but faded during the second half by his own admission. 1987/88 turned to be a joyous campaign for Liverpool but a personal disaster for Mølby. He broke his leg after a challenge by John Wark in pre-season training and In February 1988 he was arrested for a high-speed car chase, having given the police the slip. The law was waiting for him the following day, having identified the perpetrator. Six months later he was put behind bars for six weeks. Mølby had been a regular as a central defender while waiting for his trial, but now faced an uncertain future at the club. Once Mølby was released Dalglish convinced the club's Board to give him another chance at Liverpool. The Scot was a big admirer of Mølby's abilities, but couldn't help but being frustrated with him. "Jan deprived an awful lot of people of an awful lot of enjoyment by not being able to stay in shape," Dalglish said. Mølby was soon back playing in January 1989 until another injury cut his season short.
After being on the fringes of the first team in the 1989/90 Championship season Mølby became a regular starter in the second part of 1990/91. Dalglish resigned and Souness took over but Mølby kept his place and on 30 November 1991 he reminded everyone of the fantastic talent he possessed. Only three minutes had passed in Liverpool's League game against Norwich at Anfield when Mølby struck a venomous shot from 30 yards into the top corner. Souness enthused: "I think the match was worth coming to see for that goal alone." Mølby won the FA Cup for the second time in the 1991/92 season which turned out to be his last as a Liverpool regular. Injuries and subsequent lack of fitness restricted him to only 42 games in his last four seasons at Liverpool before being released in 1996.