Yossi Cohen gave details about the theft of Iran's nuclear archive.
The warehouse raid in 2018 ferried tens of thousands of documents out of the country to Israel.
He also hinted at Israeli involvement in the destruction of Iran's nuclear facility at Natanz, and the assassination of a nuclear scientist.
Cohen retired as the head of Mossad last week.
He spoke to journalist Ilan Dayan on Channel 12's Uvda documentary programme, which was broadcast on Israeli television on Thursday night.