[6] In 1952, she starred opposite Inge Egger and O. W. Fischer in Eduard von Borsody's Ich hab' mich so an Dich gewöhnt [de].

Tiller had her artistic breakthrough in the 1955 film Die Barrings, directed by Rolf Thiele,[5] alongside Lil Dagover, Ida Wüst, Paul Hartmann and Dieter Borsche.

[8] She played Lulu opposite Mario Adorf in 1962,[11] followed by Schloß Gripsholm, after Tucholsky's novel, in 1963, and Tonio Kröger based on Mann's novella in 1964.

She performed with partners such as Curd Jürgens, Hansjörg Felmy, Yul Brynner, Robert Mitchum, Rod Steiger, and Jean Marais, and at the height of her career was considered along with Sophia Loren to be among the most alluring women in European film.

[2][5][11] In 1967 and 1968, she appeared on the open stage at Salzburg Festival in the annual play, Hofmannsthal's Jedermann (Everyman), as the Buhlschaft.

After a long absence from the cinema, she was cast in 2005 by Til Schweiger in his roadmovie Barfuss, and in 2009 by Leander Haußmann in his film comedy Dinosaurier – Gegen uns seht ihr alt aus!

[5] From September to October 2010, Tiller made guest appearances in the role of the greatest diva of all time in Schorsch Kamerun's production of the play Vor uns die Sintflut at the Thalia Theater Tent in Hamburg's Hafencity.

From January – April 2015, she appeared in the musical My Fair Lady as Mrs. Higgins at the Staatstheater Braunschweig, a role she repeated in the 2015/16 season.