The 39-year-old - who split from boyfriend John Mayer last month - is playing a Fatal Attraction style stalker on the hit comedy.
At one point the actress made quite a scene on set, tackling one of her male co-stars with gusto.
She's already won over the show's star and executive producer, Tina Fey, who said: 'Jennifer is not only incredibly lovely to have around, she also has what the young people would call 'mad skills.'
Aniston, who rose to fame as Rachel on Friends, will play Fey's room mate Claire Harper in the episode.
Free-spirited Harper shows up in New York and rapidly attaches herself to Alec Baldwin's character Jack Donaghy.
The announcement that Aniston would be returning to NBC was made last week, by NBC Entertainment's executive vice president Teri Weinberg.
'She is the perfect comedic talent to work with the Emmy-winning 30 Rock cast.
'This promises to be a memorable, hilarious night of comedy.'
Aniston's last primetime TV acting role was on best friend Courteney Cox's series Dirt.
The real-life friends shared a kiss when Aniston guest-starred on the show last year.
30 Rock, which has won Emmy, Golden Globe and Screen Actors Guild Awards, returns to US TV screens on October 30.
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