In the video, posted to Instagram on Monday by the @popcultureangel account, the Australian actor, 31, looked visibly embarrassed by the Hannah Montana star, 28, as she began twerking at a Vanity Fair Oscars after-party.
The event took place just two weeks after the high-profile couple tied the knot.
In the footage, Miley twerked in front of Liam during their joint Access interview.
The Hunger Games actor quickly stepped away from his bride while looking uncomfortable.
'Don't do it. Don't do it,' he begged her. 'You're scaring everyone on the carpet.'
Miley then stopped, before glancing awkwardly at the camera.
Liam could be seen wearing his wedding ring in the video, which was recorded just six months before the A-list couple filed for divorce.
In the same Monday post, another video from April showed deepening tensions between the couple as 2019 wore on.
At the Avengers: Endgame premiere, Miley tried to pose seductively while Liam clung to her waist.
The clearly annoyed pop star pushed her husband's hands away, while he offered an embarrassed grin.
She then raised her arms and posed up a storm.
Liam and Miley filed for divorce just four months later, after being together on and off for a total of 10 years but only married for eight months.
He is now dating Australian model Gabriella Brooks.

It comes after Liam sent fans wild on Tuesday when he debuted what appeared to be 'nose ring' in an Instagram selfie.
He shared a close-up photo alongside his dog, and fans were quick to spot what looked to be a new piercing.


The actor's followers soon realised, however, it was just his dog's whisker in the frame of the photo.
'Thought you got a nose ring and almost fainted,' one fan wrote.
Another wrote: 'Thought you had a nose ring for a second...def would look greatttttttt.'
Another added: 'I thought it was a nose ring, then realised it was a dog's whisker.'