it’s so sweet to see a girl doing something like this for her guy=)
Stellar-incubus
Tonight,Tonight-Smashing Pumpkins
Closer-nine inch nails
living dead girl-Rob Zombie =D
Damn I Wish I Were Your Lover - Sophie B. Hawkins
Have to second the Chris Isaak suggestions.
How dare we get this far into a list without some Al Green!
Come Away With Me - Norah Jones, the song or the whole album.
She’s The One - World Party
Sky - Robert Fripp
Ganges Delta Blues - Ry Cooder & V.M. Bhatt
Beat The Retreat - Richard Thompson
Big Sky Country - Chris Whitley
Aerial - Chris Whitley
Grey/Afro - Skip Spence
Sanctuary - Miles Davis
The entirety of Roxy Music’s Avalon was the default option during my college days (twenty f-in years ago now, that was).
Yeah. Am I the only one who thinks that their cover of Jealous Guy is better than the original?
Anyway, as to the OP, if you really want to get a guy in the mood: Theme From “Shaft”.
I would add:
Secret Rendezvous by Karyn White
Sign Your Name by Terrence Trent D’Arby
Delicate by Terrence Trent D’Arby
Lenny by Stevie Ray Vaughan
Gawd! I feel so OLD! I don’t recognize any of the names posted so far. But if you want to set a romantic mood, almost anything by Johnny Mathis in the ‘50s is just right. Add Al Hibler singing “I’ve Got It Bad (and that ain’t good)” with the Duke Ellington Orchestra and an album of Sarah Vaughan’s silky voice and you could keep me going for, oh, ten, fifteen minutes easy. I TOLD you I wuz old. 
Cry?!?
Anti-mood setting in my opinion. Breakup songs don’t usually make for good mood setters.
You don’t know how to set the mood, you don’t know…You don’t know how to set the mood!
Now, for me, that was the only song I could sing to my son when he was a baby to make him stop crying. To me it will always be a lullaby.