Croatia star Modric completed a medical and signed a five-year contract with the Spanish champions, bringing to an end weeks of speculation about his future at White Hart Lane.
The 26-year-old, who cost Spurs £16.5m four years ago, has generated a transfer fee profit of £13.5m, plus around £3m more in possible add-ons related to appearances and success.
That cash looks certain to be spent before Friday night’s summer deadline for moves, with Tottenham manager Andre Villas-Boas eyeing two midfielders, a striker and a goalkeeper.
First to arrive could be Lyon stopper Hugo Lloris, after Spurs revived their interest in the France No1 over the weekend. The north Londoners had a £12.5m bid rejected earlier this month. Lloris, 25, is thought to want a move to a top European club, with Tottenham keen to bolster their goalkeeping options and mindful of 41-year-old Brad Friedel’s advancing years.
Villas-Boas is also monitoring Shakhtar Donetsk’s Brazilian attacking midfielder Willian, a player the Portuguese showed interest in while manager of Chelsea last season.
The Blues failed with a £17m bid for Willian during the January transfer window and, despite the premature departure of Villas-Boas, reconsidered the player this summer after Shakhtar dropped their price.
Spurs are also trailing France and Rennes defensive midfielder Yann M’Vila, a long-time target of their arch-rivals Arsenal.
Tottenham are mulling whether to raise their offer for M’Vila, 22, after a £12.5m bid was rejected. Gunners boss Arsene Wenger failed with a late raid on Rennes in August 2011 but his interest is thought to have cooled.
Villas-Boas could yet sign another striker, despite landing Emmanuel Adebayor on a permanent deal from Manchester City, with Internacional and Brazil’s Leandro Damiao top of their shortlist.