About 1400 the brothers were apprenticed to a goldsmith in Paris, and between 1402 and 1404 Pol and Jehanequin were working for the duke of Burgundy in Paris, possibly on the illustration of a Bible moralisée, now in the Bibliothèque Nationale, Paris. Some time after Burgundy's death in 1404, they entered the service of his brother, the duke de Berry, and it was for him that their most lavishly illustrated books of hours (book of hours) (the popular form of private prayer book of the period) were produced. The Belles Heures (or Les Heures d'Ailly) show the influence of the Italianate elements of the contemporary French artist Jacquemart de Hesdin's illuminations. The Très Riches Heures du duc de Berry, considered their greatest work, is one of the landmarks of the art of book illumination and ranks among the supreme examples of the International Gothic style. It is essentially a court style, elegant and sophisticated, combining naturalism of detail with overall decorative effect. An awareness of the most progressive international currents of the time, particularly those deriving from Italy, suggests that at least one of the brothers visited there. The Très Riches Heures was left unfinished in 1416 but was completed about 1485 by Jean Colombe.

The Limburg brothers were among the first to render specific landscape scenes with accuracy. Their art did much to influence the course that Early Netherlandish art was to take during the 15th century.