The special agreement wants libraries and the university to work together holding lectures, exhibitions and conferences.
Speaking to The Washington Post Archbishop Jean-Louis Brugues, the French archbishop of the Catholic Church, said: "The library was very much interested in Notre Dame helping the library to have a greater presence in the United States and to reach a larger American public."
The archbishop went on to say that when he became the archivist and librarian in 2012 he was "surprised and a bit disillusioned to discover that so many treasures within its collections that belong to the whole of humanity are not available to the whole of humanity."
He said he had worked with colleagues to find ways to get more scholars going into the Vatican Library to do research and make the most of its resources.
Archbishop Brugues said that he thought Notre Dame "was the best door to enter."
The Vatican Library was started in the 1450's by Pope Nicholas V.
It houses around 180,000 manuscripts, 1.6 million books and 150,000 prints, drawings and engravings.
Revd John Jenkins, Notre Dame's president, said the two bodies working together will be a great resource.
He said it was important for the university "to be joined with a place that is such an icon to the church's commitment to learning.
"We believe this is the first step in a number of steps to develop a relationship that will expose the great treasures of the Vatican Library to scholars and students alike," he said.