He later starred in the psychological science fiction romantic drama film Eternal Sunshine of the Spotless Mind (2004) this performance is repeatedly lauded as one of the most important and seminal in Carrey's career and for which he was nominated for both the BAFTA Award for Best Actor in a Leading Role and another Golden Globe Award.

He was also praised for his dramatic role of Jeff Piccirillo in the Showtime tragicomedy series Kidding, for which he was nominated for another Golden Globe. The Guardian named him one of the best actors never to have received an Academy Award nomination. In 2006, Carrey received a Grammy award nomination for Best Spoken Word Album for Children.

In 2013, Carrey published his first book, a children's story titled How Roland Rolls, which was awarded a 2013 Gelett Burgess Children's Book Award. In 2020, Carrey published his first novel, Memoirs and Misinformation, which he co-authored with Dana Vachon.