Eighteen English portrait miniatures from the Victoria and Albert Museum collection were analysed using Raman microscopy and optical microscopy. Most had been attributed to well-known artists such as Levina Teerlinc, Nicholas Hilliard and Isaac Oliver, but there were some of uncertain attribution. Each miniature was examined in detail in order to characterise the palette used by the artists, paying attention not only to the identity of the materials but also to the shape, size and distribution of the pigment particles. The different mixtures used in various areas, such as the carnation, used for the skin tones, lips and dark physiognomic detail helped the authors to distinguish between different miniaturists. This approach, associated with conservation, curatorial and art historical expertise, was used to suggest an attribution for three miniatures where previously the artist was uncertain or disputed. This type of analysis should be extended to a larger number of miniatures from the same period and geographical provenance in order to build up a stronger database and reach a statistically significant sample size. © 2012 Victoria and Albert Museum Journal of Raman Spectroscopy © 2012 John Wiley & Sons, Ltd.