He received his doctorate in 1927 with a dissertation on the influence of Pierre de Ronsard on French poetry (1550–1585); published shortly after, the work has become a classic (it was republished in 1965).
Raymond's subsequent study of French poetry from the end of the nineteenth century to the beginning of the twentieth – De Baudelaire au surréalisme (1933) – brought him universal critical praise.
During the Second World War, Raymond lost his father and several friends (including Benjamin Crémieux who died in a concentration camp), but he poured himself into essays, critical editions and anthologies on Montesquieu, Agrippa d'Aubigné, Victor Hugo and Paul Valéry.
His later work comprises both poetry (Poèmes pour l'absente dedicated to his wife), autobiographical works (Le Sel et la cendre, Souvenirs d'un enfant sage), fragments of a diary (Le Trouble et la présence, Écrit au crépuscule), philosophical reflection (Par-delà les eaux sombres), literary theory (Vérité et poésie, Être et dire) and studies on Senancour, Fénelon and Jacques Rivière.
In all of his work on French poetry and on Jean-Jacques Rousseau, the fundamental principle of Raymond's approach was a focus on the ways literature comes out of a contemplative discovery of the self within the world.