Keane was probably born after 1620 and before 1660, possibly around 1655. He is believed to have been a son of the second marriage of Daniel Carroll of Ballymooney.
His father was outlawed as a result of his participation in the Confederate wars, and exiled to Spain. He was attained for treason and his property confiscated.
Keane is believed to have married Mary Dillon and is thought to have had 4 children.
Keane obtained a lease for the property 'Aghagurty' from his relative Richard Grace, in 1686 and became known as Keane Carroll 'of Aghagurty', which means 'Fields of Hunger'. His half brother Daniel was made head tenant on another portion of land and was known as Daniel Carroll of Aghagurty. There was widespread famine as a result of the confiscation of property from the Irish who rebelled against the English plantations and Catholic oppression.
Keane served as a Jacobite soldier under Brigadier Francis Carroll in the Williamite wars and survived the Battle of Boyne in July 1690 when the Jacobites were defeated. He was attainted for treason in 1691 and his property was forfeited. Many of his kinsmen and thousands of his fellow Jacobites went into exile in France. In 1694 he filed for restoration of his lease under the Limerick Agreement and this was granted. However, in 1700, the trustees of the forfeited properties refused to uphold the decision, even though Keane had already paid a significant sum to settle it. In 1703 the property was sold to an English company, the Corporation of Hollow word Blades.
Keane and his wife both died before 1706, according to the details of her father's will.
Their son Daniel migrated to the colony of Maryland in 1717 when he turned 21, assisted by his cousin Charles Carroll The Settler. Daniel settled in Prince George's County, becoming a successful merchant and was known as Daniel Carroll I of Upper Marlboro.
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