The news comes after months of controversy about her salary at the charity – and the profitability of the Rehab scratchcard scheme.
A statement from the group says Ms Kerins – who has strong Tipperary connections – has sent a message to staff, outlining increasing concerns she's had recently about the toll that public controversy has taken on the group and on her own family.
She says she's dedicated her energies and ability to growing the group for 22 years, but she's of the view that it's in the best interests of all concerned that she step down.
Angela Kerins appeared before the Public Accounts Committee in February to face a grilling by politicians on a number of issues, including her €240,000 pay packet.
PAC member Mary Lou McDonald has indicated this morning that even if Ms Kerins leaves her position, they'll still be looking for answers from her.