As King William II had no sons, Albrecht was appointed the army's commander and assigned to the Ardennes, with Walther von Lüttwitz serving as his chief of staff.

Albrecht also commanded the German forces during the Second Battle of Ypres, where poison gas was used on a large scale for the first time.

The new Army Group Duke Albrecht was placed under his command in February 1917, and he was responsible for the southern sector of the Western Front until the Armistice.

Albrecht had become heir presumptive to the Kingdom of Württemberg following the death of his father in October 1917, but the German Empire's World War I defeat and the abdication of his cousin King Willhelm II of Württemberg following the German Revolution prevented him from ever succeeding to the throne.

Albrecht was married in Vienna on 24 January 1893 to Archduchess Margarete Sophie of Austria,[6] a daughter of Archduke Carl Ludwig.