After the series ended, the brothers formed a duo called Nat & Alex Wolff, and released the albums Black Sheep (2011), Public Places (2016) and Table for Two (2023).

Wolff focused his career on film roles, portraying Dzhokhar Tsarnaev in Patriots Day (2016) and John "Derf" Backderf in My Friend Dahmer (2017).

His other acting roles include My Big Fat Greek Wedding 2 (2016), Jumanji: Welcome to the Jungle (2017), Hereditary (2018), Pig (2021), Old (2021), and A Quiet Place: Day One (2024).

[11] Wolff began his acting career at the age of 6 in the 2005 musical comedy film The Naked Brothers Band: The Movie, written and directed by his mother.

Wolff made a cameo in the Nickelodeon TV movie Mr. Troop Mom and the USA police-procedural, comedic television drama Monk, both in 2009.

In 2016, he had a supporting role in the comedy sequel My Big Fat Greek Wedding 2 and played terrorist Dzhokhar Tsarnaev in the drama Patriots Day, about the Boston Marathon bombing.