Charles was a son of Landgrave Ernest Constantine of Hesse-Philippsthal (1771–1849) from his marriage to Louise (1775–1808), daughter of Prince Charles Frederick of Schwarzburg-Rudolstadt.
Charles succeeded his father as the Landgrave of Hesse-Philippsthal in 1849, after his older brother Ferdinand had died in 1839.
Charles served as a Major General à la suite in the army of the Electorate of Hesse.
After the War of 1866, Prussia annexed, among others, the Electorate of Hesse and Hesse-Philippsthal.
Charles married on 9 October 1845 in Pokój with Marie (1818–1888), a daughter of Duke Eugen of Württemberg (1788–1857), with whom he had two children: