The match, which saw Liverpool win 4-2 on the night and 5-3 on aggregate, attracted a 40% peak share of the audience at 9.30pm, as the game reached a thrilling conclusion, with three goals in the last 10 minutes.
ITV1's live coverage of the match averaged 8.6m viewers and a 35% share, while the entire programme averaged 7.5m viewers and a 31% share between 7.30pm-10pm.
ITV4's simultaneous coverage of the Champions League match between Chelsea and Turkish side Fenerbache, which Chelsea won 2-0, drew 621,000 viewers and 2.9% share. It peaked at 8.10pm with 809,000 viewers and 3.8% share.
The outcome of the two-quarter final matches is good news for ITV ratings, as it means an all-English semi-final and guarantees an English club will reach the Champions League Final for the fourth successive year.
ITV will air live coverage of the Champions League final in May but it is not known yet whether it or Sky, which shares TV rights for the competition in the UK, will broadcast the first or second leg of the all-English semi-final.
Despite the popularity of the football, Channel 4's new series of 'How to Look Good Naked' got off to strong start, with 2.6m viewers and a 10.5% share between 8pm-9pm.
Including Channel 4+1, the first episode brought 2.8m viewers and an 11.1% share.
The last episode of BBC One's eight-part comedy drama 'Hotel Babylon' pulled in 4.1m viewers and a 17% share between 9pm-10pm.
Five's 'CSI: Crime Scene Investigation' netted 2.8m viewers and an 11.5% share in the same one-hour slot.