In 2016, Simone starred in the Oprah Winfrey Network drama series Greenleaf, playing the role of Zora Greenleaf, the daughter of Kerissa (Kim Hawthorne) and Jacob Greenleaf (Lamman Rucker). Simone was originally cast as a recurring cast member but was promoted to a series regular as of the second season. Simone later made her film debut, playing the supporting role opposite Jennifer Hudson in the 2018 drama film Monster that premiered at the 2018 Sundance Film Festival.
The following year, she appeared in two drama films that premiered at the 2019 Sundance Film Festival: Share and played a leading role in Selah and the Spades. Both films have received positive reviews from critics. Later in 2019, Simone was cast as one of leads in the horror film The Craft written and directed by Zoe Lister-Jones and based on the 1996 film of the same name. She has a Youtube channel with over 11,000 subscribers.