The 'Stay With Me' hitmaker - who scooped four Grammy awards at the weekend - is a big fan of the country singer and would love to make a record with her.
Asked who he wants to collaborate with, he said:''I like Kacey Musgraves, the county singer. She's great. That would be great.''
And it seems Kacey is keen to work with the British star.
E! reporter Marc Malkin tweeted: ''I love this. @samsmithworld told me he'd love to work with @KaceyMusgraves. Let's make that happen right now. #GRAMMYS'', prompting Kacey to reply:
''@marcmalkin @samsmithworld Let's do it!''
Meanwhile, Sam ''freaked out'' at the Grammy Awards when soul legend Stevie Wonder sang one of his own songs to him backstage.
He said: ''I was in my changing room and Stevie Wonder was next to my changing room.
''He asked me to come to his room and I walked in and he started playing my song to me, 'I'm Not the Only One,' and he started singing it to me and I was like what the f**k?
''I just freaked out and got on my phone and filmed a little. It was incredible.''
His new album Underneath It All is out now.