The 38-year-old was named Mick McCarthy's assistant at the weekend as the Barnsley-born boss returned to take over the Irish national side for a second time and with his new coaching responsibilities, Keane has opted to call time on his playing career.
The veteran scored an impressive 68 goals in 146 games for his country as well as a prolific club career spanning spells at Inter Milan, Leed United, Tottenham, Liverpool and Celtic, among others.
Famed for his cartwheel celebration, Keane plundered 325 goals in 737 games during his club career.
In his statement, Keane thanked Wolves for handing him his first chance in football and insisted that he had loved every minute of his lengthy spell as a professional footballer.
"From Crumlin United around the world to the likes of Milan, London and Los Angeles, I could never have imagined the path my football life would take. It has exceeded all the hopes I had as a football-mad boy growing up in Dublin," he wrote.
"Leaving home at 15 years of age to pursue my professional career in England seems a lifetime ago now. I was a street footballer full of hope armed with huge ambitions and a determination to succeed. All I needed was that one chance.
"I have always wanted to test myself and strive to be the best that I could be, so I embraced new challenges be it at Coventry City, Inter Milan, Leeds United and then possibly the most successful period of my club football career with Tottenham Hotspur.
"I had the great privilege to represent and captain Tottenham over 238 games. I had many wonderful times there and I will look back on my days at White Hart Lane with great fondness. The club will always hold a special place in my heart.
"There were shorter times spent at Glasgow Celtic and Liverpool, two truly iconic global institutions, and then West Ham United, before Los Angeles became our home away from home. We spent five hugely successful and rewarding years, both on and off the field, with LA Galaxy.
"I enjoyed every moment of the most incredible journey with the Ireland team over an 18-year period and as I have said many times before, words cannot express how proud I am to be Irish. I hope I have made the fans proud wearing the green jersey and armband.
"With the closing of one chapter comes an exciting new adventure. I am incredibly proud, honoured and excited to now be working alongside Mick McCarthy, Terry Connor and the Irish international team over the next number of years.
"This is a role I have massive passion, energy and enthusiasm for and I hope to use my experiences to contribute towards a bright future in Irish football."