Countess Caroline of Nassau-Saarbrücken (12 August 1704 – 25 March 1774) was Countess Palatine of Zweibrücken by marriage.
She was the daughter of Count Louis Crato of Nassau-Saarbrücken (died 1713) and Countess Philippine Henriette of Hohenlohe (1679–1751).
On 21 September 1719, at the age of 15, she married her 44-year-old godfather, Christian III of Zweibrücken. The wedding took place at Castle Lorenzen in Nassau. This marriage produced four children:
- married to Landgrave Louis IX of Hesse-Darmstadt
When Christian III died in 1735, Caroline took over the Regency for five years, with the consent of Emperor Charles VI, until her son Christian IV came of age.
From 1744 to 1774 she lived at Bergzabern Castle. She died on 25 March 1774 in Darmstadt at the age of 69. Her grave is in the City Church in Darmstadt.