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Law found further critical and commercial success in Steven Spielberg's A.I. Artificial Intelligence (2001), Sam Mendes' Road to Perdition (2002), Minghella's Cold Mountain (2003), for which he earned Academy Award and BAFTA nominations, in addition to the drama Closer (2004) and the romantic comedy The Holiday (2006). His subsequent roles were as Dr. Watson in Sherlock Holmes (2009) and Sherlock Holmes: A Game of Shadows (2011), a young Albus Dumbledore in Fantastic Beasts: The Crimes of Grindelwald (2018) and Fantastic Beasts: The Secrets of Dumbledore (2022), and Yon-Rogg in Captain Marvel (2019); all of which rank among his highest-grossing releases. Other notable films include Contagion (2011), Hugo (2011), Side Effects (2013), The Grand Budapest Hotel (2014), and Spy (2015), as well as the television series The Young Pope (2016), The New Pope (2020), and Star Wars: Skeleton Crew (2024), earning a Children's and Family Emmy Award for Outstanding Lead Performer nomination for the latter.

In addition to his film work, Law has performed in several West End and Broadway productions, including Les Parents terribles in 1994, Hamlet in 2010, and Anna Christie in 2011. These earned him nominations for two Tony Awards. He has also been awarded the Honorary César and was named a knight of the Order of Arts and Letters by the French government.