He's a "monster. Hateful. I hope he rots in that jail," Onil Castro, 50, told CNN.
"I don't even want them to take his life like that," he said, referring to a possible death penalty charge in the case. "I want him to suffer in that jail."
"I feel the same way," added brother Pedro Castro, 54.
Onil and Pedro were arrested soon after their brother Ariel Castro a week ago, when the three women, and a daughter born to one of them while in captivity, were discovered at Ariel's home in Cleveland, Ohio.
In the interview, both said they had no idea what was happening.
"I don't know how my brother got away with it for so many years," Pedro said, adding he would have turned him in himself if he'd been aware.
"If I knew, I would have reported it, brother or no brother," he said.
The brothers said they never went past the kitchen in Ariel's house, where the three women were kept hostage, explaining Ariel kept the rest of the house blocked off with curtains and played the television or radio to block out sounds.
The two said they were kept separate from Ariel at the jail, but Onil saw him at least once.
Ariel said "Onil you're never going to see me again. I love you, bro," the brother recounted.
Ariel Castro, a 52-year-old unemployed bus driver, was arrested after one of the victims, 27-year-old Amanda Berry, managed to call out to a neighbor, who kicked in the door to the suspect's home and rescued her and her six-year-old daughter.
Onil said he was especially horrified because they knew the father of DeJesus and Ariel even went to vigils for the teen girl and hugged her mother.
"Felix, I know that you are out there listening, and you know that I was concerned about your daughter, and I had not even the slightest idea that this would be going on," he said, according to an excerpt posted on CNN's website.
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