Villers produced many portraits of the painter, and their relationship evolved into working together, making hundreds of images based on photographic experiments.

In 1962 Heinz Berggruen edited a book, Diurnes (Daytime), based on 30 of these images accompanied by an original text by Jacques Prévert.

Since the 1950s, Villers shot many portraits of great artists, among them: Fernand Léger, Alexander Calder, Jacques Prévert, Alberto Magnelli, Oliver Mark, Jean Arp, Le Corbusier, Salvador Dalí, Joan Miró, Marc Chagall, Max Ernst, Jean Cocteau, Bram van Velde, César Baldaccini, Hans Hartung, Pierre Soulages, Antoni Clavé, Antoni Tàpies, Francis Ponge, Luis Buñuel, Federico Fellini, Léo Ferré, Michel Butor, Ben Vautier, Henri Dutilleux, and Zao Wou Ki.

In 1984 he published his text Photobiographie recounting his life, his artistic process and his relationship with Picasso in a special issue of Les Cahiers du Sud dedicated to him.

The city of Mougins in the Alpes Maritimes honored Villers with the creation of a Museum of Photography bearing his name [fr].