Kalenberg began her career in 2001, after hearing about a casting on the radio. She appeared in two television films, Hanna – Where Are You? (Hanna – Wo bist Du?) in 2001, and In the End the Truth (Am Ende die Wahrheit) in 2002. In 2003, apart from appearing in television series Vice Squad (Die Sitte) and Tatort (Tatort), Kalenberg also made her film debut, in drama The Puppet Grave Digger (Der Puppengräber). Throughout 2004 and 2005, she acted in four television films — The Doctor (Die Ärztin), The Sting of Scorpion (Der Stich des Skorpion), Secret of the Red House (Das Geheimnis des roten Hauses) and (Kabale und Liebe). In Intrigue and Love, Kalenberg starred as Luise Miller, opposite famous German actor August Diehl.
In 2006, Kalenberg starred film The Cloud, based on the novel Die Wolke, for which she won the New Faces Award for Best Actress. She then starred the 2007 drama (Was am Ende zählt). In 2008, Kalenberg appeared in various projects on television and film, the most notably fantasy film Krabat, opposite David Kross and Daniel Brühl, and mini–series Rosamunde Pilcher – The Four Seasons (Rosamunde Pilcher – Die vier Jahreszeiten). The following year, she starred two short and two full– length films, A Song Sleeps in All Things (Schläft ein Lied in allen Dingen) and Vision – From the Life of Hildegard von Bingen (Vision – Aus dem Leben der Hildegard von Binge). The later one earned her Lilli Palmer Memorial Camera at the 2009 Golden Camera Awards ceremony.
In 2010, Kalenberg portrayed Kristina Söderbaum in film Jew Suss: Rise and Fall, winning Askania Award for Shooting Star. In 2011, she made episode appearances of television series Countdown – The Haunt Begins (Countdown – Die Jagd beginnt) and Wilsberg, and acted in film Adam's End (Adams Ende). It was announced Kalenberg would star a new television film, Löwenstein, which is expected to be released in 2012.