Ariel, Onil and Pedro Castro were arrested on May 6 after one of three women held captive for a decade, Amanda Berry, broke free through a door with the help of locals.
The footage, obtained by Cleveland news outlet WKYC-TV, reveals a noticeably upset Onil running into a glass window and smashing his head twice, as they are processed at the police station. Police initially suspected Ariel's brothers were also involved in the kidnapping of Berry, Gina DeJesus and Michele Knight.
After the outburst Onil is whisked away by police. Ariel watches on, between the brothers, only metres away.
In the half-hour video, the brothers say very little to each other, until Ariel breaks the ice briefly.
Onil, the youngest of the three, looks to be the most affected by the arrest and allegations.
The brothers were released at a hearing days later after investigators failed to find any evidence linking the pair to their brother's crimes.
Since, they have described Ariel as a "monster" and wish he "rots in jail".
"I'm just grateful they are home and out of that horrible house, and I'd just tell them I'm sorry for what Ariel done," Pedro Castro told CNN.
"I hope the world listens to us," Pedro Castro said. "You already got your monster, please give us our freedom."
On Wednesday, Ariel pleaded not guilty to 329 charges of aggravated murder, rape, kidnapping, gross sexual imposition, felonious assault and one count of possession of criminal tools.
The indictments only cover the period between August 2002, when Michele was first abducted, to February 2007.
More charges could be filed against him.
Berry, DeJesus and Knight, were abducted from the same block separately from 2002 - 2004 when they were 14, 16, and 20 years old. Each had accepted a ride from Castro
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