Di Matteo has been tasked with providing the Bundesliga club some much-needed consistency in a season that has seen them beat rivals Borussia Dortmund in the league but lose to a third-tier club in the German Cup.
"With the change in coach we want to give a new impulse," Schalke sports director Horst Heldt said in a statement. "We are absolutely convinced that Roberto Di Matteo can stabilise the team so as to reach its Bundesliga and Champions League goals.
"We are missing the necessary consistency to meet our targets. This is why we took this step," Heldt said. "The performance of the team in the past few weeks has fluctuated."
Di Matteo has limited top flight coaching experience, although he did land the Chelsea job after leading the side to Champions League success in 2012 as a caretaker manager but was fired after eight months in charge when their form dipped.
The 44-year-old former Italy international had two other managerial stints in England, coaching West Bromwich Albion and lower-division side Milton Keynes Dons.
Schalke have been struggling domestically this season and have recorded just two wins in 10 competitive games.
Despite crashing out of the German Cup in the first round, Schalke have enjoyed a relatively good start in the Champions League, drawing 1-1 at Chelsea before matching that result at home to Maribor in their second group game.
In the Bundesliga, however, Schalke are languishing in 11th place on seven points after recording just two wins, forcing bosses to act, Bundesliga rights holder Sky Television said.
Keller, who narrowly escaped the axe several times before, had been in charge at Schalke since December 2012.
(Reporting by Karolos Grohmann; Editing by John O'Brien)
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