I honestly think we'll never see a Big 4 at this point, especially the way the band has evolved over the past several years --- they're spending less time together when off of the road, Dave is largely songwriting on his own and dropping band parts in later, etc. I'm not implying that that's right or wrong, it's just different from the earlier days. I also think it's harder to draw from the song well creatively after pulling out song after song for more than two decades; further, on us, I think we've elevated the Big 3 to almost mythical status, reliving the nostalgia of our younger days, that it's harder get the same reaction to the band's music that we had years ago: see "Neural Nostalgia: Why do we love the music we heard as teenagers?"
http://www.slate.com/articles/health...rence_and.html.
I think Away From The World was the band's best shot at Big 4 status since the "Lillywhite Sessions" (Busted Stuff, I love, but it sounded a little sterile compared to those earlier scrapped sessions). Just consider Snow Outside -> Drunken Soldier and Broken Things. However, it's hard to give that album Big 4 status when 2 of the songs are effectively solo songs, Sweet and Belly Full. I also think If Only is kind of weak, even if fun occasionally to listen to.
All of that said, if they really did a nice job with some unreleased material, working with someone like Lillywhite who can properly layer their sounds, then I think you have an album that could achieve Big 4 status. Specifically:
Sweet Up And Down
The Idea Of You
Sugar Will -> Water Into Wine
Kill The King
Monkey Man
#40
Crazy Easy
Break For It
Good Good Time
Shotgun ->
Loving Wings
[Joy Ride has been released; JTR has basically been released; Can't Stop, Break Free are weak songs; Sister is effectively a solo song; Blue Water is great, but probably empty-sounding in the studio; A Dream So Real never really went anywhere; Granny would be a contender, but it's been around for so long now, I don't know, would be the next one worthy of inclusion..]