The Unforgettable, which was the couple's first LP, was an unconventional recording and it turned them into stars. The song "Baat Niklegi" from the album achieved great popularity for the Singhs. The Independent described it in 2011 as "ground-breaking ... it became a transformative, before-and-after milestone in the history of Indian popular and ghazals music. It remains that." Using modern arrangements, it consists of ten tracks that include two on which they sang as a duo and the remainder equally split between Jagjit and Chitra singing the lead. The Independent further noted that "This format of solo and duet performances from the first commercially successful husband-and-wife team in Indian popular music proved astonishingly successful." Jagjit explained that "I was determined to polish up the genre and make it more acceptable to modern tastes, so chose simple poems and set them to simple tunes. I also introduced western instrumentation to make them livelier." Thereafter, the couple worked both on solo and joint musical projects and performed concerts worldwide. There was success from involvement with the film industry and they amassed considerable wealth,.
Singh turned 70 in February 2011. To celebrate his 70th birthday he committed 70 concerts in different parts of the world. He toured the UK, Singapore, Mauritius, inter alias, in 2011 and was due to perform with Ghulam Ali in Mumbai but suffered a brain haemorrhage on 23 September 2011. He was in coma for over two weeks and died on 10 October at Lilavati Hospital, in Mumbai. He was cremated the following day at Chandanwadi Crematorium near Marine Lines in Mumbai.