As an inventor, he was interested in the fields of transmitting graphics by telegraph[citation needed] and making photographs in color, but he is perhaps best known for being the first person to conceive a method for reproducing recorded sound, an invention he named the Paleophone.

In the early 1880s, Charles Cros was a member of the Hydropathic Society and part of the fumist group led by Alphonse Allais and Arthur Sapeck [fr].

Cros's proposals, which anticipated the subtractive method of modern photography, were similar to more influential ideas advanced about the same time by Louis Ducos du Hauron.

[6] The same day, 7 May 1869, Charles Cros and Louis Ducos du Hauron presented their method of creating color photographs to the French Society of Photography.

Cros ended up conceding the invention to Ducos Du Hauron, despite having deposited a sealed paper at the French Academy of Sciences on 2 December 1867.

The English translation is one close to this: "A lightweight armature is fixed to the center of the face of a vibrating membrane; it ends with a sharp point [...] which rests on a lamp-blacked surface."

His poem The Kippered Herring inspired Ernest Coquelin to create what he called monologues, short theatrical pieces whose format was copied by numerous imitators.

Charles Cros, played by Christopher Chaplin, appears in the film Total Eclipse, about the lives of Paul Verlaine and Arthur Rimbaud.

Marie Corelli published one of his poems posthumously in the text of her 1890s' book, Wormwood, with a special note of respect to the recently deceased author.