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Craig Ross is currently Woking’s interim head coach, following the sacking of Neal Ardley, and will still be in the dugout for Tuesday’s meeting with Altrincham.
Defoe will then take over for Woking’s home clash with Eastleigh on Good Friday.
The 43-year-old will be assisted by former Fulham and Halifax manager Paul Bracewell, who played in Everton’s brilliant title-winning teams of the 1980s.
Woking said they had opted for Defoe “following a detailed recruitment process” and said his “values, leadership style and footballing philosophy best aligned with its long-term vision”.
Chairman Todd Johnson said: ”Jermain’s achievements as a player speak for themselves, but what stood out to us during the process was how he sees the game, how he drives standards, and his approach to leadership and player development.
”We have a clear plan for where we want to go as a club, and we believe Jermain is the right person to build on the strong foundations already in place and help take us forward in the next phase of that journey.”
Defoe’s 23-year professional career saw him score 305 goals in 763 senior appearances, across spells at West Ham United, Sunderland and Portsmouth, among others.
He netted 20 times for England in 57 appearances, playing at the 2010 World Cup in South Africa and Euro 2012 in Poland and Ukraine.
His task will be to guide Woking into the Football League for the first time.
The Surrey club have long aimed to recapture their glory days of the 1990s, which included a number of promotions, an unforgettable surprise 4-2 victory at West Bromwich Albion in the FA Cup, and three FA Trophy wins at Wembley.
Woking are currently in 11th place in the National League table, with seven games of their campaign remaining.
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