Angrand exhibited his work in Paris at Les Indépendants, Galerie Druet, Galérie Durand-Ruel, and Bernheim-Jeune, and also in Rouen. His work appeared in Brussels in an 1891 show with Les XX. In the early 1890s, he abandoned painting, instead creating conté drawings and pastels of subjects including rural scenes and depictions of mother and child, realized in dark Symbolist intensity. During this period, he also drew illustrations for anarchist publications such as "Les Temps nouveaux"; other Neo-Impressionists contributing to these publications included Signac, Luce, and Théo van Rysselberghe.