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His work was exhibited at the Paris Salon in 1868, 1885, and 1895. In 1889 Lerolle painted the murals The Crowning of Science and The Teaching of Science in the Hôtel de Ville, Paris. He painted Flight into Egypt in the Sorbonne, and also did works in Schola Cantorum (the establishment of which he was involved), and the church of St. Martin des Champs, both in Paris. Lerolle was made a Chevalier, Légion d'honneur in 1889.
Lerolle owned several canvases by Maurice Denis including Catholic Mystery, and is considered to be Denis's first important patron. In fact, Denis claimed that Lerolle "discovered him." In 1892 Lerolle commissioned Denis to paint a ceiling mural for his home entitled "L'Echelle dans le Feuillage" ("Ladder in the Foliage"). Additionally, Lerolle was a friend and patron to Degas and Renoir, the latter of whom painted several portraits of Lerolle's daughters and of Lerolle himself. Lerolle also owned works by Fantin-Latour (who painted Lerolle's wife, Madeleine Escudier), Corot, Gauguin, and others.
Madame Lerolle's sister, Jeanne, was married to the composer Ernest Chausson and the Lerolle home, at 20, avenue Duquesne  was a meeting place not only for artists, but also musicians of the day including Vincent d'Indy, Claude Debussy and Paul Dukas. Having met via Lerolle, Chausson also commissioned works by Maurice Denis. Lerolle was also a violinist and composer.
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