NBC said Tuesday that the show will end after 17 years, with Daly deciding to focus on other work and his family.
In a statement, Daly said it's time to hand over the show's 1:30 a.m. Eastern time slot and try something new within NBCUniversal.
He will remain a host and producer on NBC's "The Voice" and continue hosting a segment on the network's "Today."
A date for the final episode of "Last Call" and the show replacing it will be announced, NBC said.
"Last Call," which debuted in 2002, featured interviews and performances by artists including Maroon 5, Ed Sheeran and Kendrick Lamar. It will have aired 2,000 episodes when it ends, NBC said.
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