The Spaniard has been replaced by Nuno Santos, who has worked with Mourinho at Tottenham, Roma and Benfica, bringing to an end a spell that saw Llopis present for Real Madrid's last five Champions League triumphs.
Llopis first arrived in 2015 alongside Rafael Benítez and remained in his post when Zinedine Zidane took over, overseeing the goalkeeping department through the club's run of three consecutive European Cups. He left in the summer of 2018, in step with the departing Zidane, before beginning a second spell at the Bernabéu with Carlo Ancelotti's return in 2021.
During that second stint, Llopis helped Thibaut Courtois, with whom he shared a close relationship, produce some of his finest form during the 2021-22 Champions League campaign, while also preparing his eventual successors Kepa Arrizabalaga and Andriy Lunin for the 2023-24 triumph. When Ancelotti departed, Llopis remained on staff under Xabi Alonso and then Álvaro Arbeloa, but Mourinho's arrival has now brought his time at the club to a close.
Announcing his exit, Llopis wrote simply: "Incredible to live it and feel it. THANK YOU."
The message drew an outpouring of tributes from the goalkeepers he worked with over the years.
"Thank you for everything, my friend," wrote Courtois, while Sergio Mestre offered "Thank you for all your love" and Luis López wrote "Thank you for everything."
Toni Fuidias and Kiko Casilla both described him as "the best," while Kepa Arrizabalaga and Fran González responded with hearts. Andriy Lunin and Keylor Navas, two of the most prominent goalkeepers to work under him, had not yet posted their own farewells at the time of writing.
Llopis leaves having won 12 major trophies across his second spell alone, including two LaLiga titles, two Champions Leagues, a Copa del Rey, three Spanish Super Cups and two European Super Cups, cementing his standing as one of the most respected goalkeeping coaches of his generation.
His departure continues a wider overhaul of Real Madrid's technical staff since Mourinho's return, with the Portuguese manager bringing in several members of his trusted inner circle to reshape the club's backroom setup. Nuno Santos arrives having worked alongside Mourinho across three different clubs, giving the new head coach a settled and familiar voice in one of the more specialised roles within any modern coaching staff.