2004 was a critically and commercially successful year for Khan. He transformed Dreamz Unlimited into Red Chillies Entertainment, adding his wife Gauri as a producer.^[116] In the company’s first production, he starred in Farah Khan‘s directorial debut, the masala film Main Hoon Na. A fictionalised account of India–Pakistan relations, it was viewed by some commentators as a conscious effort to move away from the stereotypical portrayal of Pakistan as the constant villain.^[117] Khan then played an Indian Air Force pilot who falls in love with a Pakistani woman (Preity Zinta) in Yash Chopra’s romance film Veer-Zaara, which was screened at the 55th Berlin Film Festival to critical praise.^[118] It was the highest earning film of 2004 in India, with a worldwide gross of over ₹940 million (US$20.74 million), and Main Hoon Na was the second-highest earner with ₹680 million (US$15.01 million).^[109][119]

In his final release of 2004, Khan starred as a NASA scientist who patriotically returns to India to rekindle his roots in Ashutosh Gowariker‘s social drama Swades (meaning “Homeland”), which became the first Indian picture to be shot inside the NASA research centre at the Kennedy Space Center in Florida.^[120] Film scholar Stephen Teo refers to the picture as an example of “Bollywoodised realism”, displaying a transcendence in conventional narrative and audience expectation in Hindi cinema.^[121] In December 2013, The Times of India reported that Khan found filming the picture such an emotionally overwhelming and life-changing experience that he had still not viewed the film.^[122] Derek Elley of Variety found Khan’s performance “unsettling” as “a self-satisfied expatriate determined to bring Western values to poor Indian peasants”,^[123] but several film critics, including Jitesh Pillai, believed it to have been his finest acting to date.^[124][125] He was nominated for the Filmfare Best Actor Award for all three of his 2004 releases and eventually won the award for Swades.^[52][61] Filmfare later included his performance in the 2010 issue of Bollywood’s “Top 80 Iconic Performances”.^[126]

In 2005, Khan starred in Amol Palekar‘s fantasy drama, Paheli. The film was India’s submission for the Best Foreign Language Film at the 79th Academy Awards.^[127] He later collaborated with Karan Johar for the third time in the musical romantic drama Kabhi Alvida Naa Kehna (2006), in which he played an unhappily married man who has an extramarital affair with a married woman. The film, which featured an ensemble cast including Amitabh Bachchan, Abhishek Bachchan, Rani Mukerji, Preity Zinta and Kirron Kher, emerged as India’s highest-grossing film in the overseas market,^[104] earning more than ₹1.13 billion (US$25.62 million) worldwide.^[109] Both his roles in Kabhi Alvida Naa Kehna and the action film Don, a remake of the 1978 film of the same name, earned Khan Best Actor nominations at the Filmfare Awards,^[128] despite his performance as the titular character in Don being negatively compared to that of Amitabh Bachchan in the original film.^[129][130]

In 2007, Khan portrayed a disgraced hockey player who coached the Indian women’s national hockey team to World Cup success in Yash Raj Films’ semi-fictional Chak De! India. Bhaichand Patel notes that Khan, who had a background in the sport playing for his university’s hockey team,^[132] essentially portrayed himself as a “cosmopolitan, liberal, Indian Muslim”.^[133] Faring well in both India and abroad,^[109][134] Khan garnered another Filmfare Award for Best Actor for his performance,^[52] which Rajeev Masand of CNN-IBN considers to have been “without any of his typical trappings, without any of his trademark quirks”, portraying Kabir Khan “like a real flesh-and-blood human being”.^[135] Filmfare included his performance in their 2010 issue of the “Top 80 Iconic Performances”.^[136] In the same year, Khan starred alongside Arjun Rampal, Deepika Padukone and Shreyas Talpade in Farah Khan’s reincarnation melodrama Om Shanti Om, portraying a 1970s junior artiste who is reborn as a 2000s era superstar. The film became the highest grossing Indian motion picture of 2007, both domestically and abroad.^[104][137] Om Shanti Om earned Khan his second nomination of the year for Best Actor at Filmfare.^[138] Khalid Mohammed from Hindustan Times wrote, “the enterprise belongs to Shah Rukh Khan, who tackles comedy, high drama and action with his signature style—spontaneous and intuitively intelligent”.^[139]

Khan collaborated for the third time with Aditya Chopra on the romantic comedy Rab Ne Bana Di Jodi (2008) opposite Anushka Sharma, at that time a newcomer. He played Surinder Sahni, a shy man with low self-esteem, whose love for his young arranged wife (Sharma) causes him to transform himself into Raj, a boisterous alter-ego. Rachel Saltz of The New York Times believed the dual role to have been “tailor-made” for Khan, allowing him to display his talents,^[140] although Deep Contractor from Epilogue thought Khan displayed greater strength in the role of Surinder and weakness in the role of monologue-prone Raj.^[141] In December 2008, Khan suffered a shoulder injury while filming a small role in Mudassar Aziz‘s Dulha Mil Gaya. He underwent extensive physiotherapy sessions at the time but the pain left him almost immobile and he had arthroscopic surgery in February 2009.^[142][143] He performed a special appearance in the 2009 film Billu, playing Bollywood superstar Sahir Khan—a fictionalised version of himself, wherein he performed musical item numbers with actresses Kareena Kapoor, Priyanka Chopra, and Deepika Padukone.^[144] As head of the film’s production company, Red Chillies, Khan made the call to change the title of the film from Billu Barber to Billu after hairdressers across the country complained that the word “barber” was derogatory. The company covered up the offending word on billboards that had already been installed with the original title.^[145]