Passenger services commenced on 11 September 1879, but the Moorswater terminus was inconvenient as it was remote from Liskeard and a long way from the Cornwall Railway station on the south side of the town.

The section beyond Looe station to the quay was closed in 1916 and the Caradon line north of Moorswater fell out of use at around the same time.

In 1966 the line was due to be closed under Richard Beeching's Reshaping of Britain's Railways plan, but was reprieved just two weeks before its scheduled closure by Minister of Transport Barbara Castle.

It is also looking at simplifying the reversal of trains, considering the costs and benefits should the line be "microfranchised" separately from the Great Western Franchise, and the potential for opening a Park and Ride station at Moorswater where the goods sidings are close to the A38 Liskeard Bypass.

The majority of Looe Valley passengers travel the whole length of the line with Causeland being the busiest intermediate station.

It then descends steeply, now heading generally southwest, and passes under the Liskeard viaduct carrying the Cornish Main Line 150 feet (46m) above.

Curving right once more, the train joins the main branch line from Looe at Coombe Junction, and comes to a stand on a small level crossing.

Another level crossing is passed at Lodge, and then a short journey brings the train to St Keyne Wishing Well Halt, adjacent to the "Magnificent Music Machines" museum of fairground organs and similar instruments.

In common with most of the stations it has been rebuilt in recent years, a smart brick shelter having replaced the original wooden hut.

All distances along the line are measured from the point near the seven-span road bridge across the river where the Liskeard and Looe Railway connected with the private sidings on Buller Quay.

During the peak summer period from 20 May to 9 September 2007 three additional services were operated, including a late evening train.

In May 2019 Great Western Railway introduced an improved timetable which saw 15 trains a day run on the line Monday to Saturday and 8 on Sundays from April until October.

[2] Signal boxes were originally provided at Liskeard (at the north end of the branch platform), Coombe Junction and in a small hut at Looe.

As of December 2023[update], the line has three ground frames which are operated by the train crews:[4][5] The Looe Valley line is divided into three sections, each worked by a different method:[5] The level crossings at Lodge Farm (between Coombe Junction and St Keyne) and at Terras (between Sandplace and Looe) are both 'open' crossings with warning signals for road users.