The pair were part of Tim Sherwood's coaching team last season but the 45-year-old Englishman, who took over after Andre Villas-Boas was sacked, left the club at the end of the campaign after just six months in charge.
The duo were also wanted by Sherwood at West Brom, with the Baggies' offers to the coaches apparently a sticking point which saw the former Blackburn and Tottenham midfielder eventually reject the chance to return to Premier League management.
Mauricio Pochettino succeeded Sherwood as the new Spurs manager and the Argentine is setting up his own coaching team at White Hart Lane.
Pochettino was appointed on May 28 after an impressive stint at Southampton and has already taken assistant manager Jesus Perez, first team coach Miguel D'Agostino and goalkeeping coach Toni Jimenez to north London with him.
A statement on Tottenham's website said: "Les returned to the club in a coaching capacity in 2008, initially working with the strikers before linking up with Tim Sherwood and Chris Ramsey coordinating the Development Squad and most recently working with the first team.
"As a player, Les scored 39 goals in 146 appearances in our colours between 1997 and 2003.
"Chris joined the Club in 2004, working within our Academy set-up, before running our Under-21 side and Development Squad in conjunction with Tim and Les, stepping up to a First Team coaching role in December.
"We should like to thank them for their contribution and wish them well for the future."