The special track has been released today (March 9) on iTunes and in Sainsbury's, with all proceeds going to the charity.
The pair - who recorded the track in LA earlier this year - will also perform together live from the London Palladium for Friday's main telethon.
"'Lay Me Down' holds a very special place in my heart," Smith said.
"Not only did I perform it at the Brits, I'm now going to perform it live on the Red Nose Day show with the extremely talented John Legend, which is so exciting.
"I recently visited a Comic Relief-funded project in my hometown which supports the young LGBT community in London. I'm extremely proud that my single will help raise money for projects like this and many others in the UK and across Africa."
Legend added: "Sam is such a talented artist. We've been looking forward to working together for a while now. I'm so glad we could collaborate on such a great song and for such a great cause."
Smith has also re-recorded the solo version of his track, to serve as his next single due for release on March 15. Listen below:
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