The band are currently finishing the follow-up to 2010's Contra and plan to release it in the spring.
Speaking of the almost two-year recording process, Ezra Koenig told Rolling Stone: "Sometimes we thought maybe we were done, but it's always very apparent when you're not.
"There was a certain point where we kind of knew deep down that it didn't quite feel right. We knew it could be better.
"We tried all different ways of working, little by little, until we reached a point where we could feel awesome about every song.
"Things that we might have found boring in the past, we've started to find more fresh. This record has more piano and acoustic guitar and organ. But at the same time, that means we needed to find ways to flip it."
Rostam Batmanglij added that they needed to be "less self-conscious than ever" to complete the project.
Watch Vampire Weekend perform new song 'Unbelievers' below: