The actor, 49, made an uncredited appearance in Avengers: Age of Ultron, but will properly kick up a gear in 2018’s Infinity War.
He’ll also be back in the untitled Avengers 4 in 2019, as well as venturing elsewhere in the Marvel stable for Deadpool 2.
“I had a really good time,” Brolin told Collider of his time as Thanos.
“I’ve had a blast playing Thanos – that was one of the funnest jobs I’ve ever had.”
Brolin was also pushed on playing Cable, accepting that it could well end up being a part he comes back to time and time again.
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“We’ll call it our limited series,” he quipped. “This is our limited series.
“Going back to really fun writing. It’s a great tone, anything goes.
“It’s a really fun stretch for me to be involved in that comedic community.”
Infinity War is expected to include at least one major MCU death, and speculation was fuelled yesterday when a casting call for a funeral scene in Avengers 4 was spotted online.
Tom Holland (Spider-Man) has also hit headlines for joking that Mark Ruffalo (The Hulk) is an even worse secret keeper than him.
Avengers: Infinity War is out in April 2018 in the UK.