Alfred Pelland was born in Quebec City on 16 May 1906. His mother, Régina Damphousse, died when he was young, and his father, Alfred Pelland, a locomotive engineer, raised their three children. In school, Pellan filled the margins of his notebooks with drawings and excelled at his art classes, with little interest in other subjects. He later changed his surname to "Pellan".
In 1920, Pellan enrolled at the School of Fine Arts of Quebec. He won first prizes in advanced courses and earned medals in painting, drawing, sculpture, sketching, anatomy and advertising. He sold his first painting at the age of 17 to the National Gallery of Canada in Ottawa.
In 1926 Pellan received the first fine arts scholarship in Quebec, which allowed him to spend several years in Paris and visit Venice. He studied at the École nationale supérieure des Beaux-Arts in Paris (1926–1930), where he received a first prize in painting in 1928 (Lucien Simon's studio). When his scholarship ended he prolonged his stay in Paris till 1940 with the help of his father, often working alone while attending the Grande Chaumière, Colarossi and Ranson art academies. He won first prize at the exhibition of mural art in 1935 in Paris and rubbed elbows with the most famous artists of the time. Traveling Europe, he became "permeated by the mainstream art of the era".
Returning to Quebec in 1936 hoping to be appointed professor at the École des Beaux-Arts in his hometown, he was rejected by the jury, who found him too "modern". With the outbreak of war he again returned to Quebec in 1940 and settled in Montreal. Works he brought back with him were praised in exhibitions in Quebec and Montreal but the cubist and surrealist works were considered too avant-garde and most did not find a buyer. From 1943 to 1952 he taught at the École des Beaux-Arts in Montreal. His active opposition to the theories of Charles Maillard, the school's director, succeeded in pressuring Maillard to resign in 1944. The school then became more liberal in its approach. Pellan committed himself to an independent art, more open to universality and evolution.
During the 1940s, Pellan illustrated poetry books and designed costumes and sets for the theatre. His style matured and developed during this period. Surrealism began to attract him more strongly: his imagery became more erotic and his paintings, always vivid and striking, became larger, more complex and more textured. No longer believing in art schools, in early 1948 he co-signed Prism of Eyes, a manifesto written by Jacques de Tonnancour advocating freedom of expression in art, speaking for a group that called for art free of any ideology.