Emboldened by the success of De Ushuahia a La Quiaca, Santaolalla dedicated himself to production work, and he aimed his focus on Mexico, which was undergoing political upheaval in the late '80s. The country was suffering from an economic crisis in the 1980s, and when an earthquake struck Mexico City in 1985, killing 10,000 people, the situation there turned dire. Moreover, the presidential election of 1988 took a fateful turn when the computer the country planned to use to count votes, a brand-new IBM AS/400, suddenly crashed on the day of the election. The government publicly announced "se cayó el sistema" (the system crashed), and when the votes were tallied later, the Institutional Revolutionary Party (PRI) candidate, Carlos Salinas, was declared the winner. This was expected, for the PRI party had controlled the government for the preceding 59 years (1929-1988); however, this was the first time the vote was controversial, and consequently "se cayó el sistema" became a cynical Mexican catch phrase. In turn, the PRI party fractured, resulting in the emergence the following year of the left-wing Party of the Democratic Revolution (PRD). Moreover, the state-controlled media monopoly in Mexico began to break down around this time, and the longtime ban on rock concerts in Mexico City, enacted in 1968, also came under pressure following a government-approved Rod Stewartconcert in the state of Queretaro in 1988.
The door to Hollywood was now opened, and Santaolalla found himself fielding a series of soundtrack opportunities. First came Amores Perros (2000), released as a two-CD soundtrack for the Alejandro González Iñárritu film of the same name. The soundtrack featured original music by Santaolalla as featured in the film, and it also featured newly recorded songs from major Latin acts such as Julieta Venegas, Café Tacuba, Control Machete, Illya Kuryaki and the Valderramas, and Ely Guerra. Both the film and the soundtrack were widely praised, and a few years later Santaolallacomposed the soundtrack for Iñárritu's next film, 21 Grams (2003). Then, introduced to Brazilian director Walter Sallesby Iñárritu, Santaolalla was invited to compose the soundtrack for The Motorcycle Diaries (2004). This score won him the BAFTA Award (British Academy Award) in February 2005 and set the stage for his Golden Globe and Oscar wins shortly afterward for Brokeback Mountain (2005).
Santaolalla got the job thanks to another chance meeting, this time with Taiwanese-American director Ang Lee. Upon reading the script for the film as well as the short story by Annie Proulx upon which the film was based, Santaolallacomposed the soundtrack -- before the movie was even shot, a rare practice in Hollywood. Lee was actually able to study the soundtrack beforehand, keeping it in mind as he went about scouting locations for Brokeback Mountain, in addition to while he shot the film. Brokeback Mountain was as controversial as it was acclaimed when it opened in late 2005, and the buzz surrounding it garnered Santaolalla a lot of media attention, all the more so when he won a Golden Globe for "A Love That Will Never Grow Old," an original song of his performed by Emmylou Harris and co-written by Bernie Taupin,Elton John's longtime lyricist. An Oscar followed, this time for Best Score. The Academy Award complemented his 2005 Latin Grammy Award from the prior year, which he'd won for Producer of the Year.