He was originally intended to follow his brother's trade of baker (he was once called "un boulanger manqué" by a hostile critic), but his love of acting led him to the Conservatoire, where he entered Régnier's class in 1859. He won the first prize for comedy within a year, and made his début on December 7, 1860 at the Comédie-Française as the comic valet, Gros-René, in Molière's Le Dépit amoureux, but his first great success was as Figaro, in the following year.
He was made sociétaire in 1864, and during the next twenty-two years he created at the Comédie Française the leading parts in forty-four new plays, including Theodore de Banville's Gringoire (1867), Paul Ferrier's Tabarin (1871), Émile Augier's Paul Forestier (1871), L'Étrangère (1876) by the younger Dumas, Charles Lomon's Jean Dacier (1877), Edward Pailleron's Le Monde où l'on s'ennuie (1881), Erckmann and Chatrian's Les Rantzau (1884).
In consequence of a dispute with the authorities over the question of his right to make provincial tours in France he resigned in 1886. Three years later, however, the breach was healed; and after a successful series of tours in Europe and the United States he rejoined the Comédie-Française as pensionnaire in 1890.
It was during this period that he took the part of Labussière, in the production of Sardou's Thermidor, which was interdicted by the government after three performances. In 1892 he broke definitely with the Comédie-Française, and toured for some time through the capitals of Europe with a company of his own. In 1895 he joined the Renaissance theatre in Paris, and played there until he became director of the Porte Saint Martin in 1897. Here he won successes in Edmond Rostand's Cyrano de Bergerac (1897), which he repeated in the summer of 1898 at the Lyceum Theatre, London), Emile Bergerac's Plus que rein (1899),' Catulle Mendès's Scarron (1905), and Alfred Capus and Lucien Descaves' L'Attentat (1906).
In 1900 Coquelin toured in America with Sarah Bernhardt, appeared on Broadway, and made his only film, the duel scene from Cyrano de Bergerac with sound recording on phonograph cylinder (see also Sound film/Early steps). On their return to France he continued with his old colleague to appear in L'Aiglon, at the Théâtre Sarah Bernhardt. He was rehearsing for the creation of the leading part in Rostand's Chantecler, which he was to produce, when he died suddenly in Paris in 1909.
Coquelin was an Officier de l'Instruction Publique and of the Legion of Honour. He published:
His brother, Ernest and his son, Jean, were also actors.