The actress said that although upcoming episodes will see Caroline and Klaus spending more time together, Caroline is too conscious of his capacity for evil to consider him a real romantic possibility.
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"She's not interested at all," Accola told TVLine. "She can completely see that he's not a good person and that he's selfish and that he's done nothing but come in and ruin the lives of the people that she's loved."
Nonetheless, she did admit that Caroline finds herself intrigued by Klaus to an extent that affects her dynamic with Tyler (Michael Trevino) when he returns.
"She's still allowing him to enter her space and her environment, and there are going to be some conflicting moments that [are] brought to Tyler's attention.
"He has an accent! Who's not intrigued when someone has an accent? Come on!"
Accola went on to discuss Caroline's reunion with Tyler, suggesting that the two may take a while to feel comfortable with each other again.
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She said: "In a romantic relationship, it takes a minute to get back into that flow, that dance."
On Tyler's reaction to a Caroline and Klaus relationship, Accola explained: "He's not privy to any sort of friendship or emotional connection that Klaus would have towards Caroline.
"It's an inevitable moment in which Tyler and Klaus and Caroline are all going to be in the same room, so it will come to a head, and we will see the repercussions of Caroline and Klaus spending time together."
Accola suggested recently that Caroline and Klaus share a desire to be loved.
Morgan has hinted that Klaus could be killed off in the season finale.
The Vampire Diaries continues on Thursdays at 8/7c on The CW. It airs on Tuesdays at 9pm on ITV2 in the UK.
Watch a promo for the next episode 'Heart Of Darkness' below: