Largely self-taught, Malbone began his professional career in Providence, Rhode Island, and by age 17 he had developed a remarkably skilled technique. A man of agreeable manners who was blessed with what his close friend Washington Allston (Allston, Washington) called “the happy talent…of elevating the character without impairing the likeness 【of his sitters】,” Malbone was the most sought-after miniaturist of his day in Providence and Newport, Rhode Island; Boston; New York City; Philadelphia; and Savannah, Georgia. His career was cut short by tuberculosis.

Many of his miniatures have survived and are highly prized for their delicacy of drawing, richness of colour, and convincing characterization. He had no formal pupils, but he freely advised other artists, notably Charles Fraser, William Dunlap, and John Wesley Jarvis (Jarvis, John Wesley).