Pop superstars like Ed Sheeran, Camila Cabello and Emeli Sande were among the artists at the Concert For Ukraine.
Jamala gave an impassioned rendition of her Eurovision-winning track 1944.
And the stories of two Ukrainians were put centre stage when they were read by actors Tamsin Greig and Eddie Marsan.
Scottish violinist Nicola Benedetti accompanied the actors as they delivered the harrowing accounts of fleeing the Russian invasion.
Friday Night Dinner actress Greig read the words of Natalya, who spent three days sheltering in a basement in Kharkiv before leaving on an overcrowded train, later finding out her apartment block and university had been destroyed.
Then, Marsan voiced the words of Artem, who spent four days travelling to Romania with his traumatised children.
Benedetti's haunting performance merged seamlessly with a viral video of Ukrainian violinist Illia Bondarenko playing a folk song while sheltering in a basement, accompanied virtually by 94 other violinists from around the world.
That segment provided a sobering perspective on a night when some of the biggest names in music delivered performances that ranged from the sombre to the uplifting.
Jamala received one of the loudest cheers of the night when she held up the Ukrainian flag that she had been holding throughout her performance.
The singer herself fled Kyiv with her children at the start of the war. "It was really hard, but I am here," she told ITV beforehand.
"Thank you so much to all musicians for supporting Ukraine, for standing with Ukraine, because it's really important for us."
Her song 1944 was inspired by her great-grandmother, who was among thousands of Tatars who were forcibly deported from Crimea by Russian dictator Joseph Stalin during World War Two.
Lyrics about "fighting against all odds" took on a new resonance as Sheeran performed his hit Perfect.
"Thank you so much for coming," he told the 8,000-strong audience at the Resorts World Arena.
"It's such an important cause and I'm so honoured to be here."
He then joined Cuban-American superstar Camila Cabello to perform their duet Bam Bam live for the first time.
She said: "We're all praying tonight for the peace and the safety of the people in the Ukraine. Thank you guys so much for being a part of this super-important fundraiser."
Singer-songwriter Tom Odell performed his ballad Another Love, which has become adopted as an anthem of solidarity among Ukrainians on social media.
Welsh rock band The Manic Street Preachers resurrected their 1998 number one single If You Tolerate This, Your Children Will Be Next - a message that originally appeared on a recruiting poster for international volunteers to fight fascists during the Spanish Civil War in the 1930s.
Nile Rodgers, Snow Patrol, Anne-Marie, Becky Hill, Gregory Porter, Paloma Faith and the Kingdom Choir also appeared, some with blue and yellow backdrops on screens, and performing next to piles of sunflowers.
There was also a recorded message from US star Billie Eilish and brother and collaborator Finneas O'Connell, who sent their "support and solidarity".
The event was broadcast live on ITV and STV. As well as millions of pounds of public donations, the broadcasters donated an estimated £3m of advertising revenue. Another £250,000 was generated by ticket sales.
The event was organised in three weeks by Guy Freeman from Livewire Pictures, who told BBC Breakfast on Tuesday that the artists and others from the music and TV industries had not hesitated to donate their time.
"Everybody was just so affected by those daily pictures of refugees, displaced people, leaving everything behind, and us all feeling helpless," he said.
"And so this is what I guess we, in the live events and TV industry, can do - something like this, to try and help."
Popular Ukrainian band Antytila, whose members have become soldiers and volunteers during the war, had posted a video showing them in military uniforms offering to perform in a live link-up from Kyiv.
However, organisers said they could not include them "as we are only able to focus on the humanitarian situation, not the politics or the military conflict".
Antytila drummer Dmitriy Vodovozov told BBC Radio 5 Live on Tuesday: "I don't agree with it because we are living in war now and everything is political to us."
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