The indie quartet will first guest for the American rockers at Manchester Arena, on Friday, June 9.
But the Sheffield date, the following night, Saturday, June 10, marks their debut on the city's biggest stage and they are promising a homecoming like no other.
WATCH: The Sherlocks made the announcement exclusively with a Facebook Live stream from Sheffield Arena on The Star's Facebook page today at 12.30pm - CLICK HERE.
BUY TICKETS: Tickets for the Sheffield Arena show on Saturday, June 10, limited to four per person, priced £49.50 to £93.50, including fees. Buy in person, call the Box Office on 0114 256 5656 or visit www.sheffieldarena.co.ukThe two sets of Bolton Upon Dearne brothers - singer songwriter Kiaran Crook, and drummer Brandon, guitarist Josh Davidson and bassist Andy - also performed acoustic songs and took part in a special Q&A with Graham Walker and fans.
Brandon told us: "To go from four lads off the street who could barely play our instruments in my dad's garage, to supporting one of the biggest bands in the world in arenas is literally a fairy tale story. Its going to be a dream supporting one of the bands we grew up listening to!"
Fans expecting news of an eagerly awaited debut album are still waiting. The band are being hotly tipped by critics and fans alike to smash high into the charts.
The Sherlocks have supported the likes of The Libertines and James.
In the past 12-months BBC Introducing took them to play SXSW, the largest music festival in the world, in Texas. They notched up a second sold out show at Sheffield's iconic Leadmill and were signed by indie label Infectious Music.
Latest single, Was It Really Worth It?, was recorded at the world famous Rockfield Studios, made famous by the likes of Queen, Oasis and The Stone Roses, in Monmouth, South Wales. Watch the music video on our site - or CLICK HERE.
Most recently they sold out many of the 35 venues on their biggest UK headline including Manchester's Albert Hall, then a packed Foundry at the University of Sheffield, with support from local emerging bands Oddity Road and Sundance.
The Sherlocks play The Church in Leeds, on April 22 and will perform at Leeds Festival, on Friday, August 25, then Reading, Sunday, August 27. For more gig details and news visit www.thesherlocksmusic.co.uk.
Kings Of Leon, who have performed at the venue five times, are best known for their global hits including Sex Is On Fire, Use Somebody, Notion and Radioactive.
They have had 12 top 40 UK singles, won two BRIT Awards and four Grammy Awards. They have released seven studio albums and the last five all topped the UK chart, with most recent offering WALLS taking the top spot both sides of the Atlantic..
Tickets for the Sheffield Arena show, limited to four per person, priced £49.50 to £93.50, including fees. Buy in person, call the Box Office on 0114 256 5656 or visit www.sheffieldarena.co.ukFollow The Sherlocks on Facebook at www.facebook.com/TheSherlocksOfficial, on Instagram at www.instagram.com/thesherlocks and on Twitter @TheSherlocks