He has enacted lead roles in romance films including Deewaanapan (2001), Dil Hai Tumhaara (2002), Dil Ka Rishta (2003), Vaada (2005) and I See You (2006), action films Asambhav (2004) and D-Day (2013), thrillers Yakeen (2005) and Roy (2015), socio-political Chakravyuh (2012), crime drama Inkaar (2013) and biopic Daddy (2017). The year 2002 marked a turning point for Rampal when he was cast in Aankhen, proving to be his first commercial success. His other commercially successful films include Don (2006), Om Shanti Om (2007), Housefull (2010), Raajneeti (2010), Ra.One (2011), Kahaani 2: Durga Rani Singh (2016) and Nail Polish (2021).
Rampal made his acting debut in Rajiv Rai's Pyaar Ishq Aur Mohabbat (2001) opposite Sunil Shetty, Aftab Shivdasani and Kirti Reddy. Rampal gave a show stealing performance and earned all the attention. He earned critical acclaim for his performance in the movie. Taran Adarsh of indiaFM wrote "Pyaar Ishq Aur Mohabbat is a showcase for Arjun Rampal to exhibit his talent. The guy looks dashing and emotes with utmost sincerity. He's handled the emotional moments with maturity, which is so rare for a first-timer. A confident debut!" This established Rampal as a leading actor in the Indian film industry. He was nominated for the Filmfare Award for Best Male Debut but swapped the awards in the Best Male Debut category at the Star Screen and IIFA ceremonies.
His next release was Ashu Trikha's Deewaanapan, in which Rampal was paired with Dia Mirza. He earned critical acclaim for his performance, but the film flopped at the box office. Taran Adarsh of IndiaFM wrote: "Arjun Rampal carries the film on his broad shoulders and comes up with a sincere performance that is consistent throughout. He is wonderful in action sequences and springs a pleasant surprise in the emotional moments by delivering the apposite expressions." Ashish Magotra of Rediff gave negative reviews on Rampal, writing: "Among the actors, Arjun Rampal as the hero does pretty much what he has been known to do. He models. His acting capabilities leave a lot to be desired." His last release of the year was Ashok Mehta's Moksha. It was actually his first film, but was released after Pyaar Ishq Aur Mohabbat. Rampal was paired with famous actress Manisha Koirala in a lead role in Moksha. This film marked Rampal's third consecutive flop at the box office, but Rampal earned critical acclaim. Taran Adarsh of IndiaFM wrote: "Arjun Rampal excels in a role that was difficult to portray. He takes giant strides as a performer and proves that he's an actor with an amazing range." Priyanka Bhattacharya of Rediff considered the movie to be "more a 70-mm portfolio for Arjun Rampal than a story."
Rampal established his own production company Chasing Ganesha Films with his wife Mehr Jesia. The first movie under that banner I See You was Rampal's last release of 2006. He played a lead role opposite newcomer Vipasha Agarwal. The movie was shot entirely in London, England. Like his past movies, I See You was also a failure at the box office and received poor reviews. However, Rampal earned critical acclaim for his work. Taran Adarsh wrote: "I See You rests on Arjun's shoulders. Arjun is efficient in a role that doesn't really demand histrionics. He has proved his credentials in the past and his performance in this film is at par with his earlier works. He works best in the dramatic portions."
2010 would go on to become the most successful year of Rampal's career with three back to back hits. The first was Sajid Khan's comedy film Housefull, in which he starred in a supporting role. The film received negative reviews, but became a huge hit at the box office. Rampal's next release was Prakash Jha's multi-starrer Raajneeti. Rampal received critical acclaim for his supporting role of Prithvi in the movie. Taran Adarsh wrote: "Arjun is a revelation and what a terrific performance he pitches in. He's like an untamed lion." His performance earned him a nomination for the Filmfare Best Supporting Actor Award. He won the award in the Best Supporting Actor at the IIFA, Apsara and Zee Cine categories. His last release of the year was Siddharth Malhotra and Karan Johar's We Are Family, in which he played a lead role opposite Kajol and Kareena Kapoor. It was an average grosser and Rampal's first successful movie that featured him in a lead role. Taran Adarsh wrote: "Arjun continues to surprise. Rock On!!, Housefull, Raajneeti and now We Are Family indicates the growth of this actor. He handles the emotional moments well, too."
In 2011, Rampal played the titular negative role in Anubhav Sinha's science fiction movie Ra.One. The movie became a successful film in India and overseas and received mixed reviews. Rampal's new bald look earned him a lot of appreciation and popularity within the audiences. Majority of the fans considered his "Ra. One" look to be better than that of the protagonist "G.One". He earned critical acclaim for his villainous performance. Martin D'Souza praised Rampal's performance and considered him to be the saviour of the film that was being flawless in the second half. He wrote: "It's only after the interval that the plot meanders a bit, loses it sting and almost falls apart like a pixelised image, before Arjun lights up the screen." Arthur J Pais of Rediff.com wrote: "The best person to gain from the film directed by Anubhav Sinha with more inane and crude sexual jokes than in any recent Hindi film, is Arjun Rampal. His body language and brooding face creates a quietly menacing villain." Raja Sen wrote: "Arjun Rampal is the best thing in the biggest budget Indian feature of all time." Aseem Chhabra considered Rampal to be the "most interesting element of the film."
Adesh Shrivastava's musical score does boast of a couple of songs that hold popular appeal, mainly the title track and 'Bhangda Paale Goriyaan'. Another highpoint of the film are its skilfully executed action sequences (Abbas Ali). Cinematography (Suhas Gujrathi) is up to the mark. The stunning locales of New Zealand have been captured brilliantly on celluloid. 2b1af7f3a8