To study the nature of ancient and modern pottery it is necessary to be able to determine the concentrations of the major constituent elements. For such studies, mass balances calculated from these elemental concentrations cluster around 100% for a silicate-silica matrix and around 80–90% in highly calcarious pottery which has a silicate-carbonate (silica) matrix. This work requires experimental measurements with coefficients of variation wihtin approximately ±5%. The high concentrations of silicon in pottery may reasonably be determined by neutron activation analysis using the nuclear reaction29Si(n, p)29 Al. Aluminium-29 has a half life of 6.56 minutes and a γ-ray energy of 1272 keV. Epithermal neutron irradiations of samples in cadmium foil are required to minimize the quantities of thermal neutron induced radionuclides. The method of analysis developed for the low flux SLOWPOKE reactor is described and the accuracy and precision of the technique is discussed by allusion to analyses of standard reference materials. The application of this technique to two different archaeological problems is addressed. The first is a case of carbonate dilution found in neolithic pottery from Iran and the second case is a problem of silica dilution in Roman pottery from Germany.