The 35-year-old revealed that he hopes the Original vampire will express his feelings for Elena (Nina Dobrev) at some point on the CW series.
"I know it's a little obvious in the world of Vampire Diaries, where everyone falls in love with Elena, but I agree that Elijah sees something beautiful in her," Gillies told The Insider.
"I would love for him to express that to her before he goes," he continued. "I feel like Elijah would be most drawn to her because she's living a better life than people who've lived for centuries longer.
"I think that's the sort of thing he's attracted to," Gillies insisted. "Even it was just a moment, I'd love to see them share something - but I think it should be more."
Gillies recently returned to the CW series after he was resurrected by Damon (Ian Somerhalder).
Joseph Morgan, who plays Klaus, said in December that he would love to see a battle between his character and Elijah.
The Vampire Diaries airs on Thursdays at 8/7c on The CW.