In 1608 Louis Frederick came to England with Benjamin von Buwinckhausen to return his father's insignia of the Order of the Garter and visited Scotland, where he was hosted by Andrew Melville of Garvock.

Louis Frederick received the possessions on the left bank of the Rhine (Montbéliard, Riquewihr and Horburg) with full sovereignty.

During the Thirty Years' War, his territory suffered badly from starvation and the plague.

His tenure as regent was dominated by conflicts with Emperor Ferdinand II, after Württemberg lost about a third of its territory due to the Edict of Restitution.

The marriage produced three children: After Elisabeth Magdalena's death, Louis Frederick married on 15 May 1625 with Anna Eleonora (1602-1685), daughter of Count John Casimir of Nassau-Weilburg (1577-1602).