Turner is believed to have started learning guitar because of the band that was one of his main influences, Oasis. Turner has always been the band's main songwriter, and his observations of inner city England have drawn comparisons to The Streets' Mike Skinner. However, Turner has admitted that during the early days of the band "nobody wanted to admit they wrote [the lyrics] so we kept trying other singers so they'd do it for us." Despite enjoying songwriting, Turner shied away from acknowledgment because he "didn't want to have piss took out of [him]!" However, he has suggested that he has always enjoyed songwriting and that since getting his guitar, has spent most of his spare moments penning new lyrics, as "that’s what [he]'d feel comfortable doing. Describing the manner in which he constructs his lyrics, Turner says

"I'll think about something and I'll be writing, penning something down and I'll keep building on that. The best stuff comes when I’ve got a melody and a rhythm so I know how many syllables each line is going to have and then build it up from there, and make it a whole thing, and try and pay attention to every aspect."

They recorded their smash hit album in August 2005 (Whatever People Say I Am, That's What I'm Not) shortly after securing their first record deal.

In August 2007 plans were announced for Turner to record an album with Miles Kane and producer James Ford. Kane, of Arctic Monkeys support act The Rascals, announced the project on 2 August 2007. The project features Turner and Kane sharing vocal, guitar and bass duties with Ford playing drums. Owen Pallett also features on the album. The duo have called themselves The Last Shadow Puppets, the album is called The Age of the Understatement, and was released on the 21 April 2008 and reached the number one spot in its first week. They recently did a small tour backed by the London Philharmonic Orchestra, starting at Portsmouth Guildhall on 19 August 2008.

Turner worked with Dizzee Rascal on the song "Temptation" from Dizzee Rascal's album Maths and English. He also worked with Dizzee Rascal on a different version of the same song "Temptation Greets You Like Your Naughty Friend" which featured on the "Brianstorm" single. Turner also features in the Reverend and the Makers song "The Machine" and features on guitar in the song "The Machine" from their debut album The State Of Things, on which he also co-wrote some of the songs with McClure. NME reported that Turner was working with Alison Mosshart of The Kills which has now been revealed to be 'The Fire And The Thud' which appeared on Humbug with Alison providing vocals. He appears on Tony Christie's album Made in Sheffield, playing "Only Ones Who Know". In October 2008, Turner made his debut as a short story writer, performing spoken word track "A Choice of Three" on his bandmates' compilation Late Night Tales: Matt Helders.

For the turn of 2009, Turner was first spotted with his sunburst finish Fender Jazzmaster at the Big Day Out festival in Australia. It also appeared that instead of using the Fender Vibroverb and the Selmer Zodiac 30, Turner had used the Selmer alone. Turner also modified his pedalboard slightly, getting rid of his Danelectro Reel Echo and his Hughes & Kettner Rotosphere MK2 and replacing them with a Boss DM-1, and a Cornell First Fuzz. He also used his Morley footswitch to switch between his amp channels and his Line Selector to guitars and organs.

In summer 2009 he used an Ovation Viper on songs from the debut album while using his Fender Jazzmaster on newer songs; he still used his Gretsch on "If You Were There, Beware". Since the release of Humbug, Turner has left organ/keyboard duties for 505 and many other newer songs (as well as guitar sections a few older) down to the new live member of the band, John Ashton. His pedalboard had changed too, it consisted of Boss Delay Machine DM-1, Morley Footswitch ABY, MXR Micro Amp, Ibanez Tubescreamer Ts-808, Coopersonic Valveslapper, Boss Chromatic Tuner, Electro Harmonix Holy Grail Plus and Electro Harmonix Hum Debugger. On the late 2009 tour he added a Fender Blender and a Morley Power Wah which he used to play the intro of Dance Little Liar.

Turner's first guitars were believed to be a black Mexican standard Fender Stratocaster guitar (As seen in the "Fake Tales of San Francisco" video), and later a Fender Olympic White American standard Stratocaster, both sporting maple fretboards. During the Whatever People Say I Am, That's What I'm Not-era Turner's pedalboard consisted of two Pro Co Rat 2 distortion pedals, Boss TU-2 tuner and a Danelectro Reel Echo played through either a Orange AD30T or Vox AC30 CC2X amplifiers. .

However, whilst touring Favourite Worst Nightmare, he replaced both his stratocasters with a black Fender Bronco with a black pickguard and rosewood fretboard - a guitar discontinued by Fender - and his ProCo pedals with an Ibanez Ts-808 Vintage Tubescreamer overdrive pedal. He also extended the pedal board with a Hughes & Kettner Rotosphere MK2, a Morley Footswitch and a Boss LS-2 Line Selector to go between his Selmer and Fender. Turner then added an Electro Harmonix Memory Man on his pedalboard used by his friend Miles Kane on 505 and Plastic Tramp live performances.

During live performances of "If You Were There, Beware", Turner still uses a Gretsch Spectra Sonic baritone and a Martin F-65 on Da Frame2R and 505.