She first learned of “The Parisian Woman” two years ago, when a shared entertainment lawyer brokered a coffee date between her and the Tony-winning director Pam MacKinnon. Ms. Thurman had always meant to return to the theater, and she was finding quality film roles thin on the ground. (Asked about a lack of great parts for women over 35, Ms. Thurman pounced before the question was finished: “Or under 35,” she said.)

She wanted to know what Broadway had to offer. And not just Broadway, Ms. Thurman said. “Any theater.”

Over coffee, she and Ms. MacKinnon batted a few classical heroines back and forth. Then Ms. MacKinnon mentioned Mr. Willimon’s script, inspired by “La Parisienne,” an 1885 play by the minor French writer Henry Becque melding boulevard comedy and daring realism. Mr. Willimon, an Off Broadway playwright before creating “House of Cards,” had relocated it to the ethics-optional Beltway of present-day D.C.

Ms. MacKinnon sent the script, and Ms. Thurman felt instantly drawn to Chloe, the Parisian woman of the title. (Chloe is actually American. Long story.) She admired Chloe’s “emancipation and her sense of entitlement, of sexual freedom,” she said. “The sheer confidence of the character.”

Chloe is a flirt and a schemer, a dilettante and a high-heeled brawler, a woman of appetite.

Another coffee date was arranged, this time with Mr. Willimon, who described the meeting as a “hey, let’s get to know each other to make sure that we don’t hate each other’s guts.” Ms. Thurman brought the script, already studded with questions and notes.

An earlier version of the play had its premiere at South Coast Repertory in 2013, featuring Dana Delany, a lower-wattage star, as the lead. But speaking with Ms. Thurman, Mr. Willimon had an uncanny feeling, “as though almost impossibly I’d written the play for her — her poise, her charm, her sense of playfulness and humor. All those things that Chloe needs in order to exist, Uma has naturally.” The play’s producers felt the same way, delaying an industry reading until Ms. Thurman recovered from a bone-breaking horse-riding accident.