"I would do anything," Brosnahan reiterated on Sunday.
"I would go crazy," Sterling then replied with a big smile, clearly excited at the prospect.
When Turner asked, "Can we broker a deal right here, right now for this?," Brown was completely game.
"I'm in, I'm in," he said as he and Brosnahan shook hands. "Deal."
Not surprisingly, the 28-year-old actress was thrilled.
"Sterling is incredible, and can clearly do no wrong," she gushed. "Everytime I see Sterling in something else ... I would follow Sterling to the end of the Earth."
"It goes both ways," Brown added.
The 42-year-old actor later shared why he's such a fan of the critically acclaimed show created by Amy Sherman-Palladino.
"The show is done at such an incredibly high level," he said. "It's so funny, and it's so full of heart. It's so specific. Like, I love the specificity of the world, and I would love to step in that. The Palladinos are so clear in what they're doing. You know, that's the type of people you want to work with."
Last week, when asked about any actor or actress she was hoping to land in upcoming episodes, Brosnahan told ET, "I love Sterling K. Brown so much."
"We treat our guest stars well!" she added, making a pitch to the This Is Us star.