The Last Shadow Puppets star laid down his signature vocals on the chorus and spoken word at the end of song with the grime group - comprised of Dream Mclean, Wallace Rice and Alex Osiris - which he described as having a "killer mix of rap and Beatles vibe".
Speaking about the new tune, Alex from Monster Florence said: “’Picture Frame’ was an accident waiting to happen.
"I came in with the idea for the song and chorus and did a demo with myself and Tom.
"The same day, we had Miles in for a writing session and asked him if he wanted to have a go at the chorus?
"He smashed it of course and that was that ... we got the verses finished and tracked and the song was done."
And 'Cry On My Guitar' musician Miles added: “Basically when I heard the demo, to me it was the best song I had heard from the lads; killer mix of rap and Beatles vibe, it’s fresh and grabs you.”
Meanwhile, the scouser previously teased that his upcoming fourth solo album is a "samba-y Motown thing".
Following the release of his indie pop single 'Blame It On The Summertime', Miles teased that his follow-up to 2018's 'Coup de Grace' will continue in the "glam vein" of its predecessor, but the 34-year-old rocker has also been influenced by Brazilian Samba music and Motown's R&B/soul artists.
He said: "It was a perfect transition from the last album to hint at maybe where we're going, but it probably could have still fitted on that last record.
"It was just a cool tune ('Can You See Me Now') and we've been writing a lot of tunes that are still in that glam vain and now we're exploring with a bit more of a - well, lately we're getting into that samba-y Motown thing. Combined into a new song. [Blame It On The] Summertime isn't really like that but I guess it's a bit Motown-y.”
‘Picture Frame’ is out now on all major streaming services.