He won a Nobel Prize in Chemistry in 1963 with Karl Ziegler for work on high density polymers.

During this time he began using crystallography to elucidate the structures of a wide variety of molecules including phosphine, arsine and others.

In 1938 he took over as the head of the Department of chemical engineering at the Politecnico di Milano university, in a somewhat controversial manner, when his predecessor Mario Giacomo Levi was forced to step down because of racial laws against Jews being introduced in Fascist Italy.

In 1935 Natta married Rosita Beati; a graduate in literature, she coined the terms "isotactic", "atactic" and "syndiotactic" for polymers discovered by her husband.

By 1963, his condition had progressed to the point that he required the assistance of his son and four colleagues to present his speech at the Nobel ceremonies in Stockholm.