The deal, which is OpenAI’s biggest acquisition, will bring in Mr. Ive and his team of roughly 55 engineers and researchers.

Jony Ive is renowned for crafting a meticulous product design aesthetic that shaped the tech cultural zeitgeist during a 27-year career at Apple.

The dueling announcements say a lot about what are arguably the world’s two foremost AI companies: Google’s models may be technically superior and more widely deployed, but OpenAI is kicking everyone...