Born to a poor family in Shkodër, Simoni was ordained a priest on 9 February 1961. He was arrested in 1967 at the time of the Albanian Cultural Revolution and imprisoned in Spaç Prison. An international symposium in May 2000 revealed the extent of the persecution, torture, and violence suffered there, which he compared to the Mauthausen concentration camp. He documented the persecutions from 1944 to 1990 in his book Martirizimi i Kishës Katolike Shqiptare (1944–1990), which was translated into Italian.
On 25 April 1993, Simoni was appointed titular bishop of Bararus and auxiliary bishop of Shkodër. The titles were bestowed personally by Pope John Paul II on Simoni and three other bishops who had survived the communist period.[2] On January 20, 2004, the Pope allowed him to resign. He was a member of the Episcopal Conference of Albania.