Much like her sister, Lorelei is attempting to win the heart of Thor. She is utterly ruthless and often calls on Loki to help her In her goals. In Agents of S.H.I.E.L.D., She is shown to be extremely arrogant and extremely determined on her goals.
Her initial appearance was in the ending of the episode "T.A.H.I.T.I.". She is teleported to the middle of Death Valley, California, where she soon finds a service station. There she finds a newlywed man and using her abilities, she is able to seduce him into driving her away from the "Valley of Death".
She later appears in the next episode, "Yes Men", along with the same man. The two stop at a roadside gas station, where a biker gang is also stopped. She then abandons the first man and seduces Rooster, the leader of the gang. She uses Rooster's bar as a hideout so that her biker minions can bring treasures and riches to her. During this time, Sif is transported to Midgard on the hunt for Lorelei. When Sif and the S.H.I.E.L.D. agents arrive at the bar, Sif attempts to confront Lorelei, but she bends the wills of the men to fight the Asgardian warrior. As Sif fights, Lorelei exits through the back door, where she encounters Grant Ward. After one touch, he is under her spell and the two ride away to Las Vegas.
She is pleased with Ward more than her former lackeys, but he realizes she does not reciprocate feelings for him. After the two become intimate together, Grant vows to kill Sif. While Coulson, Sif, and May are busy tracking Lorelei and Grant to the hotel, they are busy sneaking onto the bus. While there, she begins controlling Fitz to incapacitate Skye and Simmons. Ward attempts to jettison Sif from the plane through an airlock in her room, but she is able to hold on and reenter. She fights Lorelei and in the end, is able to outfit her with the collar that prevents the sorceress from speaking and manipulating male victims. After the Bus lands, she is transported back to Asgard with Sif to face Odin's wrath.