"I have enjoyed every moment of my time with Wales. Everyone knows how passionate I am about my country," Hartson added on the Welsh FA's official website (www.faw.org.uk)
Hartson had been part of manager Chris Coleman's backroom staff throughout the qualifying campaign for the 2014 World Cup.
Despite finishing second from bottom in Group A there were some positives for Hartson and the Wales camp as they claimed two 2-1 wins over Scotland, both times coming from a goal down.
They finished strongly last month by taking four points from two games including a draw at group winners Belgium.
Former Arsenal striker Hartson's decision to stand down comes at a time of uncertainty for Wales with Coleman, who has been linked to the vacant manager's job at his old club Crystal Palace, yet to sign a new contract with the FAW.
Wales next play a friendly at home to Finland on November 16.
(Writing by Mark Young, Editing by Ken Ferris)
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