He had his first solo album RAAG Time in 1991-92.The song from his latest album Kisi Din 'Teri Yaad' was the title track'Jab Chandani Barh Kar' of his first album. In 1994, he composed music for a film for the first time. The Pakistani film, in which Adnan was the lead with his wife Zeba and famous Indian playback singer Asha Bhosle did the playback, Sargam, was a blockbuster. However, the authorities banned Asha's voice from the soundtrack which disappointed Adnan. He then had to re-record these songs with Hadiqa Kiyani. After unsuccessfully trying to make it to the competitive Pakistani pop scene in 1997, in 2000, Asha Bhosle teamed up with him to release a collection of love songs named Kabhi to Nazar Milao. The music was also composed by Adnan. According to Adnan, this was a "dream come true" for him. The album became an instant rage and topped the Indipop charts for most of 2001. According to BusinessWeek, the album sold 2 million copies in India.

Songs Kabhi to Nazar milao whose music video featured model Aditi Gowitrikar and Lift karaa de whose music video starred the popular Bollywood star Govinda from the album became immensely popular at this time. The videos were shot by Anil Mehra who had shot popular Hindi movies Hum Dil De Chuke Sanam and Lagaan. Looking at the immense success of this album, Magnasound and Adnan released an album Always yours which is a remix version of numbers from this album.

He soon became a "sensation" which led Hindi filmmaker Boney Kapoor to invite him to give music for his film. This was the beginning for him composing and singing songs for Hindi films very successfully of even the top Hindi film producers of the time like Yash Chopra and Subhash Ghai. Due to the immense popularity of his music videos and live performances, he had even begun getting acting offers at this time.

The song, Tu sirf mera mehboob, from the Hindi movie Ajnabee (2001) sung by Adnan also "became a rage" and was a superhit.

Screen called him the pop personality of the year 2001 and even says that the success of his album Kabhi to Nazar milao "kept the Indian pop music industry alive and breathing" in 2001.

In 2002, Pepsi Foods made Adnan its brand ambassador in India, a contract which involved hosting a series of live music concerts across cities as well as Adnan featuring in ads for Pepsi products. According to the Pakistani newspaper Dawn, no Pakistani artist had managed to gain as much popularity in India as Sami had. According to an article in the Indian newspaper The Times of India, Sami was the most successful face in non-film music in India at that time.

His second studio album, Tera Chehra, was released in October 2002 to critical eulogies even as his first album was still selling. The music videos for this album were shot by Binod Pradhan who had shot the popular Hindi movie Devdas, directed by Bela Sehgal (director of Devdas Sanjay Leela Bhansali's sister) and featured popular Bollywood stars Rani Mukerji in the title track, Amitabh Bachchan in the track Kabhi nahi who also sang the duet with Adnan and actress Mahima Chaudhry in another song. The title track was written by famous Hindi movie lyricist Sameer. According to Screen, it was the only successful pop album of the year.

Saathiya (2002) brought the opportunity to work with maestro A. R. Rahman in the form of Aye Udi Udi which he was looking forward to. According to Screen, the song was the highlight of the album. rediff.com called him the "reigning king of Indipop" in early 2003 based on the sales of his albums in the past two years.

His most successful albums have been Kabhi To Nazar Milao (with Asha Bhosle) and Tera Chehra, and his music videos usually have had a host of Bollywood stars in them, including Namrata Shirodkar ("Bheegi Bheegi Raat"), Mahima Chaudhry, Raveena Tandon, Rani Mukerji ("Tera Chehra"), Govinda, Fardeen Khan, Amisha Patel ("O Meri Jaan"), Bhumika Chawla ("Maahiya"), Dia Mirza ("Pal Do Pal") and most famously, Amitabh Bachchan ("Kabhi Nahi"). and in 2007 the soundtrack from the hit Salaam-e-Ishq: A Tribute to Love.

Since 2003, he has sung for a few Tamil movies like Boys, Aayutha Ezhuthu composed by A.R. Rehman. The songs,"Boom Boom" from Boys and "Nenjamellam Kadhal" for Aayitha Ezhuthu, were hits. He also sang for the Tamil and Telugu versions besides the Hindi version of songs fromthe movie Yuva (2004) whose music was also composed by A. R. Rahman. Besides Rahman, he also worked together with composer Yuvan Shankar Raja, singing hit Tamil songs "Oh Intha Kadhal" from Satham Podathey and the very recently released "Oru Kal" from Siva Manasula Sakthi, which got very popular and widely noticed.

In 2006, he took a sabbatical, and reportedly lost over 70 kg, to make a comeback in April 2007 with a new album Kisi Din.