In 1884 and 1886 Angrand participated in the Salon des Indépendants, and, in 1889, in the exhibition of Belgium avant-garde group Les Vingt in Brussels. The death of his friend Seurat in 1891 was a great blow for Angrand. He moved to Normandy and led a solitary life there, even stopped painting for some time.
Up to 1900 his painting of form became increasingly pointillist; In 1900 he set for experimenting with big rectangular brush-strokes. Unlike points they did not create the optic unity, their main advantage of them was intensity of color. Later he returned to an almost traditional technique with simple forms. Angrand participated in the Salon des Indépendants in irregular periods until his death. In his political views Angrand supported Anarchism, took part in illustrating Anarchist publications and helped them financially.