Manchester-born Crolla was a heavy 100-1 underdog prior to the fight.
A two-time Olympic gold medalist from Ukraine, the 31-year-old Lomachenko was expecting to face IBF champion Richard Commey until a broken right hand for Commey brought on a change of plans. After the fight, Lomachenko called out Mikey Garcia, who will likely return down to 135 after losing to Errol Spence Jr.at welterweight last month.
Lomachenko has retained his WBO and WBA lightweight titles after the one-sided bout at the Staples Center.
Lomachenko (13-1, 10 KOs) continued his historic march, which includes titles in three weight divisions, by flooring Crolla face first in Round 4 with a ideal right hook to the side of the head to cap off yet another one-sided performance.
Lomachenko then showed why it was a bad idea for Crolla (34-7-3), whose toughness wasn't enough.
And he is targeting "historic" fights, with WBC lightweight title holder Garcia in his sights.
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"I've been doing this for well over 50 years, and I've never seen anything like that guy", said Bob Arum, Lomachenko's Hall of Fame promoter.
"I want Mikey Garcia, (but) I want to unify titles", Lomachenko said.
"It will be very historical, a big fight".
The Ukrainian delivered a devastating knock-out in the fourth round at the Staples Center in Los Angeles to continue his remarkable legacy as the pound-for-pound star of the sport.
As the fight continued, Lomachenko was relentless with his attack and opening up with his offense while Crolla simply shelled up and was attempting to survive the onslaught.
In the co-main event, longtime super middleweight champion Gilberto "Zurdo" Ramírez remained unbeaten when his light heavyweight debut against Tommy Karpency was stopped by Karpency's corner before the fifth round.