Crowds swarmed in and around stations Wednesday afternoon and early evening, trying to get on trains before they stopped running around 6 p.m. (1 p.m. ET). The strike is scheduled to end Thursday night.
Some 4 million journeys are typically made on the Underground each day, so when the system is down, the city comes close to grinding to a halt.
Without the trusty Tube, as the Underground system is widely known, commuters and tourists alike were forced to find their way to their destinations by bus, train, bicycle, taxi or on foot.
A time lapse video posted to Instagram on Wednesday showed commuters climbing over the walls surrounding the steps of the Oxford Circus station to try to catch the last trains home.
Abbie Morrow posted a photo to Instagram showing the clogged streets of London as seen from her view on an hour and 15-minute bus ride.
For those who preferred to trust their own feet, Britain's Independent newspaper tweeted an image of a pedestrian-friendly map showing walking times between stations.
John Thumwood, 64, a systems consultant who works in the center of London, took the strike in stride while riding home on a packed, exceedingly hot subway train late Wednesday afternoon. He planned to work virtually Thursday, even if he'd have to cancel some meetings.
"When you're living in London that long, you just have to learn to live with it," said Thumwood, a native of the English capital.
Then he paused and added, "Of course, I think it's bloody inconvenient."
Mayor: Londoners 'understandably furious'
Extra buses and river boat services were lined up in anticipation of the strike, according to Transport for London, the body that oversees public transit across the city. But all services and the road network were expected to be very busy.
Speaking on phone-in radio station LBC on Wednesday, London Mayor Boris Johnson said residents were "understandably furious" about the strike.
"The thing is ridiculous, and it is not a well-founded strike," he said, adding that he hoped "common sense will prevail."
The strike action was called after unions and the London Underground failed to agree on a pay deal over a new "Night Tube"
service due to start in September.
Beginning September 12, when the Night Tube rolls out, there will be round-the-clock service on part of the network on Fridays and Saturdays, meaning shift workers and late-night revelers will find it much easier to get home.
But the unions say London Underground has done too little to meet its members' concerns about pay, health and safety, working conditions and promises about job cuts.
Union: We want a 'sensible solution'
One of the four unions involved in the negotiations, the Transport Salaried Staffs' Association, blamed "intransigence" on the part of London Underground for the strike action going ahead, despite months of talks.
"We work to keep London moving day in, day out. We're already often at work before 5 a.m. or can be found helping passengers get home safely in the early hours. We cope with an ever-increasing numbers of passengers -- 100 million more in just the last five years -- and are happy to do so," said a statement on the TSSA website
"We don't object to working these hours, or the even longer ones due to the Night Tube. All we ask for is a sensible solution to the safety implications of the Night Tube, honest negotiations and a reasonable settlement on pay and hours."
Johnson, on the radio show, said that the Night Tube was "something that millions of people have wanted for a long time" and that Underground workers had been offered "a very, very fair deal" in exchange.