Mother of one of the terrorists of the Students Islamic Movement of India (SIMI) was also arrested along with the four.
The three-hour-long operation involving an exchange of fire was conducted jointly by the police forces of Odisha and Telangana.
The SIMI members, wanted by NIA and several states, were arrested from a house in the steel city after an operation launched on the basis of intelligence inputs, Odisha Director General of Police K B Singh said.
Mohammad Aijajudden, Mohammad Aslam, Amjad Khan, Zakir Hussain Sadiq, Mehboob Guddu, along with Faisal, the leader of the gang, and another prisoner, had made an audacious escape from the district jail in Khandwa in Madhya Pradesh after scaling a 14-foot wall.
While the seventh prisoner surrendered the next day and Faisal was caught in December 2013 from Barwani in Madhya Pradesh, the five others evaded police.
Aslam was killed in an encounter with Telangana Police on April 5, 2015 but there was no clue of the remaining four.
The group is suspected to be involved in a bank robbery in Karimnagar (Telangana) on February 1, 2014, blast in a Bangalore-Guwahati train at the Chennai Central station that killed a young software engineer, on May 1, 2014 and the July 10, 2014 explosion near Faraskhana and Vishrambag police stations in Pune.
They were also allegedly involved in explosions in Roorkee in Uttarakhand and in Bijnor in Uttar Pradesh.
A 12-year-old boy was killed in the blast at the rally in Roorkee on December 6, 2014 while the December 14, 2014 explosion in Bijnor took place when the SIMI members were mixing chemicals with Improvised Explosive Device (IEDs).
The SIMI activists had been staying at Rourkela the past two years by using a false identity, police said.
Five guns and some ammunition were seized from their hideout.
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