The One Direction heartthrob has become smitten with the 22-year-old actress after watching her collect the Best Actress Oscar at the 85th Academy Awards last Sunday and is now "begging" mutual friends to introduce them.
A close pal of Harry's told the Daily Star newspaper: "He fell in love with Jennifer after watching her speech at the Oscars. Harry likes goofy girls and thinks it's hilarious that she fell over as she went to accept her award for Best Actress.
"And obviously, like most men, he thinks she's drop-dead gorgeous. He's been begging mutual friends who know Jen to put the word out for him so they can hook up next time they're in the same city.
"Harry is quietly confident because he normally gets whichever girl he sets his sights on."
A source said: "Nothing actually happened between them that night - there were too many people about. But there was some pretty serious flirting going on. She and Harry plan on meeting up at this weekend or next week.
"They are talking about hitting a few clubs. It's obvious they are keen to see each other again but they won't want it to look like a date."