Tom Holland's career as an anime voice actor consists of a single, notable role. He provided the voice for the character Sho in the English-language version of the 2010 Studio Ghibli film The Secret World of Arrietty. This part marked his debut in film, which he secured at the age of fifteen following his early success on the London stage in the musical Billy Elliot.

The Secret World of Arrietty, directed by Hiromasa Yonebayashi, is an animated fantasy film based on the novel The Borrowers. In the story, Holland's character Sho is a twelve-year-old boy who moves to his aunt's house in the countryside to rest before a hospital operation for his heart condition. While there, he discovers a family of tiny people, known as Borrowers, and forms a friendship with the young Borrower girl, Arrietty. In his performance, Holland portrayed Sho with a reserved and gentle demeanor, using soft tones to reflect the character's frailty, a contrast to the more energetic roles he would later play. Holland himself noted that the experience of voice acting for animation was technically challenging, requiring precise timing to synchronize his voice with the animated character's movements, but he expressed that he thoroughly enjoyed the process.

While his role in The Secret World of Arrietty is his sole credit in anime, it is often cited as the beginning of his screen career. This experience preceded his later work in other forms of voice acting, such as his roles in the animated films Spies in Disguise and Onward.