The four hailing from Maharashtra and one from Dakshina Kannada in Karnataka were arrested two days ago in connection with the robbery, Police Commissioner Jyothiprakash Mirji told reporters here.
Police also recovered Rs 32.15 lakh, gold ornaments worth Rs 3 lakh, a gun which was stolen from the security guard and vehicle used for committing the crime.
The five were remanded in 14-day police custody, he said.
About seven to eight members of the same gang were absconding and would be nabbed soon as "we have definite clues about them", Mirji said, expressing confidence about recovering the remaining cash also.
On May 14, personnel belonging to a security agency were transporting money belonging to Corporation Bank to the ATMs in their vehicle, when they were waylaid and attacked by a 14-15 member gang. After injuring the security guard sitting in the vehicle, the gang sped away with the vehicle with Rs 1.91 crore cash.
Mirji said all the five accused hatched the conspiracy to commit the robbery in Arthur Road prison (Mumbai) where they had served a jail term for three years from 2005.
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"The accused also held meetings after being released from jail and were watching the movement of the ATM van for about three to four months before they decided to strike," Mirji said.
The gang was also involved in various such crimes in Maharashtra and Mulki (Dakshina Kannada), the officer said.