Officers have also interviewed two further people in relation to events at St Francis Boys' Home in Shefford, Bedfordshire.
A 72-year-old unnamed man was arrested on suspicion of sexually assaulting four children whilst a 79-year-old man, also unnamed, is accused of six sexual and 14 physical assaults.
It's claimed the abuse happened at the home in the 1960s and 70s.
Police have identified more than 80 potential victims of alleged abuse at the home.
A 68-year-old woman and a 78-year-old woman were interviewed under caution for sexual assault but both released with no further action.
A Bedfordshire Police spokesman said: "At the conclusion of the interviews a report will be submitted to the Crown Prosecution Service."
St Francis Boys' Home has been described by former residents at the "orphanage from hell".
Several allegations have been made against Fr Wilfred Johnson, who ran the home between 1945 and 1954 and Fr John Ryan, who ran the home in the 1960s. Both men are now dead.
The Roman Catholic Diocese of Northampton has previously said it "deeply regrets" any hurt caused but stressed the "claims are not proven".
Both men arrested have been bailed pending further inquiries.
