Born in Kassel, Charlotte was the seventh child and fourth (but second surviving) daughter of William V, Landgrave of Hesse-Kassel and his wife, Countess Amalie Elisabeth of Hanau-Münzenberg.

[5] Due to his princely position and church belief, Charles I Louis couldn't get a divorce without Charlotte's consent, although he tried again and again in vain despite her disobedient, stubborn, morose and unruly demeanor.

Unlike her ancestor Christine of Saxony, who in 1540 accepted the morganatic second marriage of her husband Philip I, Landgrave of Hesse (who subsequently fathered children with both women), Charlotte strictly refused to this.

Charles I Louis, as the owner of the highest executive and judicial power in the Electoral Palatinate, finally on 14 April 1657 decided to unilaterally and officially divorce his wife and proclaimed this publicly.

Charlotte initially didn't return to Kassel after her "divorce" but lived in a wing of Heidelberg Castle, still hoping that her marital bond could be restored.

Sophia, who had lived at the Heidelberg court for a few years prior to her marriage, had seen it enough: she hated and despised her sister-in-law and was happy to help her brother take her daughter away from Charlotte, presumably to persuade her to return to Kassel.

[5] There are two touching letters from Charlotte to her daughter from the time she was traveling to Hanover, and several others to her tutor, in which she inquired about the child's condition and complained that she was no longer getting an answer.

[10] After Marie Luise von Degenfeld died in 1677 following complication from her 14th pregnancy, Charles I Louis tried in vain to obtain the consent of his first wife to an official divorce so that he could marry again equally and ensure the succession of the Electoral Palatinate, since the marriage of his eldest and only legitimate son, the Electoral Prince Charles with Princess Wilhelmine Ernestine of Denmark had been childless for seven years.

After the death of her son on 26 May 1685, Charlotte retired to an apartment in Neuburg Abbey, where she lived on a meager pension; however, she continue to visit Heidelberg Castle, where she died ten months later, on 26 March 1686 aged 58.