The 30-year-old Love and Other Drugs actor had previously said Portman was the Audrey Hepburn of our generation.
In response, Natalie, 29, told Access Hollywood at yesterday's Screen Actors Guild Awards: 'Well, he is the Cary Grant of our generation.'
Speaking about Jake, she added: 'He is so charismatic.
'And so dapper and smart. He is wonderful.'
The Closer actress was referring to the English-American actor who is known for his roles in To Catch A Thief and None But The Lonely Heart.
Natalie continued to receive praise for her peers after she received a SAG Award for Outstanding Actress, for her role as a ballerina in Black Swan.