He was born at Ancy-le-Franc into a noble family, the son of Antoine d'Ailleboust and Suzanne Hotman.

After being named governor in 1648, he tried in vain to prevent the Iroquois from annihilating most of the Hurons, who had allied themselves with the French settlers.

On 17 May 1657, at Saint-Nazaire, Paul Chomedey de Maisonneuve and d'Ailleboust, as well as three Sulpicians (Gabriel Souart, Antoine d'Allet, and Dominique Galinier) under the leadership of Gabriel de Queylus,[1] the first superior of Saint-Sulpice at Montreal, boarded the ship bound for Canada.

In the middle of August the four Sulpicians, whom the Jesuits had kept as their guests for a few days in their residence, settled down at Ville-Marie.

He was buried on 1 June 1660, in the cemetery of the hospital that stood on the site of today's Place d'Armes.