It is thought that Martini was a pupil of Duccio di Buoninsegna, the leading Sienese painter of his time. According to late Renaissance art biographer Giorgio Vasari, Simone was instead a pupil of Giotto di Bondone, with whom he went to Rome to paint at the Old St. Peter's Basilica, Giotto also executing a mosaic there. Martini's brother-in-law was the artist Lippo Memmi. Very little documentation of Simone's life survives, and many attributions are debated by art historians. According to E. H. Gombrich, he was a friend of Petrarch and had painted a portrait of Laura.
Simone was doubtlessly apprenticed from an early age, as would have been the normal practice. Among his first documented works is the Maestà of 1315 in the Palazzo Pubblico in Siena. A copy of the work, executed shortly thereafter by Lippo Memmi in San Gimignano, testifies to the enduring influence Simone's prototypes would have on other artists throughout the 14th century. Perpetuating the Sienese tradition, Simone's style contrasted with the sobriety and monumentality of Florentine art, and is noted for its soft, stylized, decorative features, sinuosity of line, and courtly elegance. Simone's art owes much to French manuscript illumination and ivory carving: examples of such art were brought to Siena in the fourteenth century by means of the Via Francigena, a main pilgrimage and trade route from Northern Europe to Rome.
Simone's other major works include the Saint Louis of Toulouse Crowning His Brother Robert of Anjou (1317, now Museo di Capodimonte, Naples); this work was painted during a stay in Naples at the request of the king. During this stay, putative pupils were his son Francesco, Gennaro di Cola, and Stefanone.

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