He graduated from the Tokyo Higher Industrial Art School in 1916.
In 1956, he was designated as a Living National Treasure by the Japanese government for his katazome stencil dyeing technique. A leading member of the mingei movement founded by Yanagi Sōetsu, Serizawa visited Okinawa several times and learned the Ryūkyū bingata techniques of dyeing.
His folk-art productions included kimono, paper prints, wall scrolls, folding screens, curtains, fans, and calendars. He also produced illustrated books, including Don Quixote, Vincent van Gogh and A Day at Mashiko.
In 1981, the Municipal Serizawa Keisuke Art Museum was opened in the city of Shizuoka. Another museum, the Serizawa Keisuke Art and Craft Museum was opened in 1989 in Sendai.
He belonged to the Kokugakai Art Society.