It includes correspondence from literary and political figures including Nobel laureate Seamus Heaney, actor Daniel Day Lewis and peace activist Una O'Higgins O'Malley relating to his work.
A native of Ballyhaunis, Co Mayo, Jordan has published biographies on prominent public figures including former prime minister of the UK Sir Winston Churchill, former president of Ireland Éamon de Valera and painter and writer Christy Brown.
Highlights from his archive include manuscripts of several books on William Butler Yeats, Maud Gonne and Major John MacBride.
There's also material relating to Major John MacBride, on whom Anthony Jordan has written extensively, including correspondence with members of the MacBride family and others.
And material relating to Christy Brown, including ‘The Guiding Light’, an early play by Christy Brown, transcribed by his brother in three notebooks, and a substantial number of letters from Christy Brown’s family and friends.
It will also include documentation relating to the National Association for Cerebral Palsy (NACPI), Enable Ireland, the Samaritans and Sandymount School and Clinic of which Mr Jordan was Principal from 1973 to 2001.
Mr Jordan said: “The Library is an invaluable national cultural institution and an essential site of knowledge and learning, one which I have taken advantage of for many years so I feel it is a fitting home for my archive.
"Some of my most exciting moments of research occurred in the NLI, and I hope that my manuscripts, and the correspondence that has informed my work, inspires future readers and researchers.”
Director of the NLI, Dr Sandra Collins, said: “Through Anthony Jordan’s work, generations of readers have gained insight into figures who have shaped modern Irish society and culture.
"We’re delighted that he has chosen to donate his archive to the National Library where it will be preserved and accessible for generations to come.”