After being denied entry into École des Beaux-Arts, he moved to Paris in 1882, where he began teaching mathematics at Collège Chaptal. His living quarters were near Café d'Athènes, Café Guerbois, Le Chat Noir, and other establishments frequented by artists. Angrand joined the artistic world of the Parisian avant-garde, becoming friends with influential members including Georges Seurat, Vincent van Gogh, Paul Signac, Maximilien Luce, and Henri-Edmond Cross. His avant-garde artistic and literary contacts influenced him, and in 1884 he co-founded Société des Artistes Indépendants, along with Seurat, Signac, Odilon Redon, and others.