They are suspected of smuggling drugs and weapons and causing serious bodily injuries, police said on Wednesday.
"Nineteen persons, whom we link to a high-level dangerous organized criminal group, were detained simultaneously early in the morning," Andžejus Roginskis, deputy chief of the Lithuanian Criminal Police Bureau, said at a news conference.
"The operation was a success: all the people were detained, no incidents occurred," he added.
Police confirmed that Giedrius Janonis, the suspected leader of the gang, was among those detained in Kaunas.
"We have received thanks from Europol, from other colleagues, for disbanding what was one of the most dangerous gangs. It was known not only in Lithuania, but also in Europe. Their activities spanned several European states," Lithuanian Police Commissioner General Linas Pernavas said at the news conference.
It is thought that, among other things, the gang committed property crimes in Germany.
More than 100 searches were conducted during the operation, which involved 300 police officers.
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