The former Tottenham Hotspur midfielder played under Mourinho for one season at Real Madrid before the Portuguese sealed a return to Stamford Bridge in June 2013.
Mourinho snapped up former Arsenal captain Cesc Fabregas in a £26.3m deal from Barcelona in June, but it appears the Chelsea boss initially wanted to sign Modric.
“I called Modric only privately but he doesn’t want [to join] Chelsea,” Mourinho told Croatian newspaper Sportske Novosti.
“You know I really appreciate Luka Modric and his qualities. But he stays in Real Madrid.”
Modric helped Real Madrid win their tenth European Cup crown last season, scoring two goals and making nine assists in 45 appearances in all competitions.
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