One of the founders of the New Primitivism cultural movement in his hometown of Sarajevo, he was also the lead singer and co-author for one of former Yugoslavia's best known bands, Zabranjeno Pušenje (No Smoking).
Karajlić also co-created and participated in TV shows Top lista nadrealista (The Surrealist Hit Parade) and Složna braća.
The name was supposed to recall the wartime practice of Partisan conspirators from World War II, who were lionized in state-sponsored movies and television series.
His deliberately low-brow and unkempt style were paired with a similar philosophical streak of New Primitivism that the band claimed to follow and propagate.
Band's pre-show press conferences often assumed the form of a debate club with Nele charming journalists while pontificating on issues ranging from lower league soccer to Karl Marx's Manifesto.
As far as on-stage behavior goes, dr Nele Karajlić was probably the first Yugo rock frontman to take a truly active approach while in front of a crowd.
Over the next seven years Zabranjeno Pušenje recorded three more studio albums and played countless sold-out arenas until, in late 1991, Nele and Davor Sučić (aka "Sejo Sexon") decided to go their separate ways.
Having written lyrics and music for most of the songs, the duo was running the band while rest of the group employed a revolving door policy.
Their already complex working-business friendship-relationship was further burdened by their ethnic background – Nele is a Serb while Sejo is identifying himself as a Bosnian, although of Croatian descent.
He could be seen across town waiting in lines in front of different charity organizations like ADRA to send food packages to family members in Sarajevo which was under siege by Serbian forces.
His first post-original-Zabranjeno Pušenje music gig was a low-publicity duet with Toni Montano on a quickly forgotten track called "Srećna porodica".
In September 1995 he traveled to Toronto where he met up with Mladen Pavičić 'Pava', formerly of Plavi Orkestar, and some local musicians, including drummer Boris Daich and bassist Nenad Stanojevic, for a Zabranjeno Pušenje show.
On the strength of their Belgrade success the new band embarked on a mini-tour across SR Yugoslavia, Macedonia, Bosnia and Slovenia during which they played some memorable arena gigs in Novi Sad, Skopje, Banja Luka and Ljubljana.
Finally in 1997, the Belgrade fraction of Zabranjeno Pušenje (of which Nele was the only original member) released Ja nisam odavle (I'm not from around 'ere) which did very well commercially in Serbia even if reviews weren't as glowing.
In the 2001 documentary Super 8 Stories legendary Joe Strummer, clearly at a loss for words, describes their sound as "this crazy Greek-Jewish wedding music of the past,... and the future".
A second one that started in the spring of 2000 saw them pay visits to cities in France, Spain, Portugal, Germany and of course Italy, which had by this time become their business base.
Kusturica's role is that of a Trojan horse – his starpower draws people to shows, he then does his talking bit at the beginning and in-between some songs (often purposely delivered in broken English) and finally turns the audience over to Nele & Co.
In May 2005 they played a show in Cannes, France, during the film festival for a movie industry crowd including Salma Hayek and Javier Bardem.