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Alois was born in Würzburg, the fifth child and only son of Karl, Prince of Löwenstein-Wertheim-Rosenberg and his wife, Carolina dei Conti Rignon. He had four older sisters, Maria (wife of Joseph, Archduke of Austria), Josephine (wife of Alexander, Prince of Liechtenstein), Monika (wife of Don Jaime Mendez de Vigo y del Arco) and Christiane (wife of Michael, Archduke of Austria), and two younger sisters, Elisabeth-Alexandra (wife of José Maria Trénor y Suarez de Lezo) and Lioba (wife of Moritz Eugen, Prince of Oettingen-Oettingen and Oettingen-Wallerstein). He and his sisters spent their childhood in Bronnbach, and Alois attended school in Miltenberg.
Alois married Anastasia (b. Brieg, 14 February 1944), the elder daughter of Prince Hubertus of Prussia, in a civil ceremony in 1965 in Bronnbach, and in a religious ceremony a month later in Erbach. The couple lives at Kleinheubach castle. They had four children:
Hubertus Maximilian Gabriel Louis Franz Constantin Dominik Wunibald Maria (born 1968); married to Iris von Dornberg
Christina Maria Johanna Caroline Magdalene Osy Cecilie Hermine Isidora Victoria Anastasia (b. 4 April 1974, Frankfurt). She married Guido von Rohr (b. 27 September 1969, Hanover) on 5 October 2002 in Kleinheubach. They have four children.[citation needed]
Dominik Wilhelm Christian Nikolaus Sturmius Antonius Charles Benedikt Felix Maria (born 1983); married to Olga zu Castell-Rüdenhausen[citation needed]
His heir apparent is his grandson, Nicodemus, born 2 August 2001.