Jake Gyllenhaal has agreed to star in a one-night-only performance of “Sunday in the Park With George” to raise money for New York City Center.

Mr. Gyllenhaal, although best known as a film star, wowed musical theater fans last summer with his star turn in an Encores! Off-Center production of “Little Shop of Horrors” at City Center. And “Sunday in the Park,” with music and lyrics by Stephen Sondheim and a book by James Lapine, is one of the most beloved shows in musical theater. The show, a look at the artistic and romantic compromises faced by the painter Georges Seurat, won the Pulitzer Prize in 1985.

The concert performance is being produced by Jeanine Tesori, the Tony-winning composer of “Fun Home,”.

The gala, honoring the philanthropist Adrienne Arsht, is scheduled for October 24; performance-only tickets will be sold for $75 beginning at noon on May 25 at nycitycenter.org.