Officials seized over 94,000 bitcoin from Ilya Lichtenstein, 34, and his wife, Heather Morgan, 31.
The seizure shows that law enforcement can follow money through the blockchain, the DOJ said.
The videos have been taken down on YouTube, but remain shared on Twitter.
That anonymity has attracted criminals, with bitcoin and the like often being used as black market currency.
However, crime accounted for less than 1% of cryptocurrency transactions last year.
Around 25,000 bitcoin – today worth about $1 billion – were transferred out of his wallet.
The remaining 94,000 bitcoin are what was seized Tuesday.
