"Heartseeker" fits Orianna's character more than "Sweetheart". Here's an excerpt from her lore:
"She tries in earnest to fit in with those around her. However, no matter how hard she tries, Orianna can never be human and there is always something unnerving and alien about her."
Does that excerpt not imply that Orianna is seeking for a human heart? Not only does she fit the title, she also fits the implications of the title, albeit slightly less well. Orianna is searching for face-to-face interactions with humans, a very human action, and one of the precursors to love. Furthermore, judging by her in-game quotes, Orianna is very active and, perhaps most importantly, deadly.
"I know what makes them tick. I know how to make the ticking stop." -Taunt
Yeah. Not a "Sweetheart" at all.