Sie war eine Urenkelin von Wilhelm von Oranien (1533-1584), wie auch ihr Gatte ein Urenkel von jenem war. Das erste Kind aus ihrer Ehe, ihr Sohn Karl, geboren am 10. April 1651, den sie sehr liebte, war sehr oft krank. Sie hatte ihm den Spitznamen "Karellie" gegeben. "Charles Louis [ihr Gatte] much preferred the healthy girl born in the following year [am 27. Mai 1652]. The pleasantest passages in his letters to his mother were those in which he dwelt with paternal pride on the charm and liveliness of his daughter Elizabeth Charlotte - "Liselotte". (in: Carola Oman: Elizabeth of Bohemia, id., pp. 378-379). Das dritte Kind, ein weiterer Sohn, der den Namen Friedrich erhalten hatte, lebte nur ein Jahr, vom 12. Mai 1653 bis zum 13. Mai 1654.
Sophie von der Pfalz berichtet in ihren Memoiren über ihre Schwägerin Charlotte von Hessen-Kassel Folgendes: "She was very tall, with an admirable complexion and most beautiful bust. Her features were irregular, and her eyebrows, which were dyed black, struck me as forming too violent a contrast with her beautiful flaxen hair; besides, in raising them she gave a kind of twist to her high forehead which had a very odd appearance. To make up for these defects she had beautiful sparkling eyes, full pouting lips, and very fine teeth; altogether she would be called a handsome woman. … It was from a weakness of mind, and not from any evil design, that she loved to attract attention. There was more folly than evil in her; but the Elector, having great delicacy of feeling, wished her to be all in all to himself and nothing to others [er war sehr eifersüchtig] … The Electress [Charlotte von Hessen-Kassel] likes hunting and cards …" (in: Memoirs of Sophia, Electress of Hanover: 1630-1680, id., pp. 36/40-41)
Charlotte und ihr Gatte wurden am 14. April 1657 geschieden. Ihrer Schwägerin Sophie von der Pfalz erzählte sie, "... she had been forced by her mother to accept 'a jealous old man' [Karl I. Ludwig von der Pfalz] , when she might have had her enamoured cousin, Duke Frederick von Württemberg-Neustadt, the attractive Dukes George and Ernest Augustus of Brunswick Lüneburg, Philip, Palsgrave of Sulzbach, 'and several counts'. ... But his temper [Karl I. Ludwig] had never been sweet, and he had begun to suffer from rheumatism. His learned sister nicknamed him after Timon of Athens, the misanthrope. Appalling stories of the scenes at his court reached the Hague. The Electress Palatine [Charlotte] had thrown a dish at her husband during dinner, whereupon he had boxed her ears. After seven years of domestic strife, Charles Louis's wife left his court for ever." (in: Carola Oman: Elizabeth of Bohemia, id., pp. 393-394).