Joao Felix remains the biggest transfer during Diego Simeone's time as a manager at Atletico Madrid.
The Portuguese attacking midfielder arrived from Benfica for a fee of €127.2m in the summer of 2019.
He scored 34 goals in 131 appearances across a four-year spell before departing for Premier League side Chelsea.
Julian Alvarez is in second in place following his €75m move from Manchester City in August 2024.
The acquisition of the Argentina striker narrowly eclipses the €72m fee that Atletico paid to sign Thomas Lemar from Monaco in 2018.
The top five is completed by Diego Costa and Antoine Griezmann, while England midfielder Conor Gallagher also features in the top ten.
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