Officials also charged two people on Tuesday with attempting to launder the money, stolen by a hacker who breached a cryptocurrency platform in 2016.
The hacker allegedly made off with nearly 120,000 Bitcoin. Then valued at about $71m, its value now exceeds $5bn.
About 94,000 Bitcoin have been recovered.
Assistant Attorney General Kenneth Polite Jr said the seizure was proof the government "will not allow cryptocurrency to be a safe haven for money laundering or a zone of lawlessness within our financial system".
The money originates from the 2016 hack of a crypto exchange known as Bitfinex.
According to Justice Department officials, a hacker breached the platform, made more than 2,000 unauthorized transactions and then funneled the money into a digital wallet allegedly run by Ilya Lichtenstein, 34, of New York.
A criminal complaint alleges Lichtenstein and his wife, Heather Morgan, 31, laundered about 25,000 of the stolen Bitcoin through various accounts over the past five years and used various methods to cover their tracks, from fake identities to converting their Bitcoin into other digital currencies.
Investigators from Washington DC, New York, Chicago and Antioch, Germany collaborated on the lengthy probe.
In a statement, Bitfinex said it had cooperated with the inquiry and was "pleased" the stolen funds had been recovered.
Lichtenstein and Morgan will appear before a federal judge later on Tuesday, on counts of conspiracy to defraud the US and conspiracy to commit money laundering.
If found guilty, they could each serve up to 25 years in prison.
The asset seizure comes four months after the launch of a National Cryptocurrency Enforcement Team at the Justice Department.
In what is believed to be its previous largest financial seizure, the team seized some $2.3m in cryptocurrency last year, recovering the ransom paid by the Colonial Pipeline company to end a crippling cyberattack.
It says police could strike a "huge blow" by targeting key services used to launder cryptocurrency by criminals.
The company previously estimated criminals received a record $14bn in cryptocurrencies in 2021.
The UK's National Crime Agency (NCA) told the BBC, law forces are responding.
Chainalysis says it tracks cryptocurrency wallets controlled by criminals such as ransomware attackers, malware operators, scammers, human traffickers, dark net market operators, and terrorist groups.
By following flows of cryptocurrency from addresses associated with criminal activity, Chainalysis was able to estimate the amount "laundered".
It says most cryptocurrency is laundered through a limited number of services - for example, particular exchanges favored by criminals - and shutting these could have a big impact.
The report notes that "while billions of dollars' worth of cryptocurrency moves from illicit addresses every year, most of it ends up at a surprisingly small group of services, many of which appear purpose-built for money laundering".
It adds: "Law enforcement can strike a huge blow against cryptocurrency-based crime and significantly hamper criminals' ability to access their digital assets by disrupting these services."
According to an Europol report, also published on Wednesday, criminal networks specialized in large-scale money laundering "have adopted cryptocurrencies and are offering their services to other criminals".
And Gary Athwart, head of financial investigation at the NCA, said: "Whilst the vast amount of cryptocurrency use and exchange is for legitimate reasons, organized criminals have identified the benefits that cryptocurrency provides them.
"There are parts of the cryptocurrency structure that are being exploited to launder criminal cash, particularly from drug dealing. The growing menace of ransomware also utilizes cryptocurrencies as its payment mechanism.
"Law enforcement is responding to this adoption by criminal gangs, and cryptocurrency seizures are increasing. Legislative changes are also being progressed to assist with the response to cryptocurrencies being used in illicit finance practices."
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