Chitons are marine molluscs that mineralize their teeth by the process of matrix-mediated biomineralization. The teeth develop in a continuous manner forming hard minerals, including magnetite, making analysis of the matrix within these mineralized regions difficult. This article describes the use of charge contrast imaging techniques, rarely applied to biological samples, to simultaneously image the organic and mineral phases within the teeth of these animals. Resulting evidence demonstrates the power of this technique in delivering architectural information concerning both the matrix and mineral phases, without the need for removal of the hard mineralized material. SCANNING 31: 11–18, 2009. © 2009 Wiley Periodicals, Inc.