The much-travelled Serb, who guided Red Star Belgrade to the European Cup in 1991, replaces former Bulgaria midfielder Krasimir Balakov, who resigned following Litex's early Europa League exit on Friday.
"Ljupko Petrovic needs no introduction," Litex president Trifon Popov told a news conference. "He has worked with us, he has proven himself in Europe. We needed an experienced coach and I think he's the perfect option."
The 68-year-old Petrovic coached more than a dozen of clubs in Serbia, Spain, Uruguay, Greece, Austria, China, Croatia, United Arab Emirates, Kazakhstan and Rwanda.
He also led Litex's rivals Levski Sofia to the title in the Bulgarian top flight in 2001.
"Litex are still a very good team and I accepted the invitation without even thinking," Petrovic said. "My goal, as always, is to win the league title!"
Petrovic won the Bulgarian Cup during his first spell at Litex in 2004 and he also coached the Lovech-based club between 2005 and 2007.
Litex host champions Ludogorets on Saturday in the opening round in the domestic league.
(Reporting by Angel Krasimirov; editing by Sudipto Ganguly)
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