This chapter examines the major element, trace element, and isotope geochemistry of the Thera pyroclastics, and places it in the context of the geochemical evolution of the whole volcanic field. Geochemical studies to date have been undertaken predominantly on the lavas, and the pyroclastic succession has been relatively neglected. The data on the pyroclastics are taken from Druitt (1983), Mellors (1988), Pyle (19906), and Edwards (1994). Wholerock analyses and sample descriptions are given in Appendix 2. Most analyses are of a single pumice or scoria lump, although some are combinations of several small clasts and a few are compositionally banded. The rock classification scheme used throughout the memoir is shown in Fig. 6.1. Previous isotopic studies on Santorini are also largely confined to the lavas, and no detailed studies had been carried out on the pyroclastic rocks. In this chapter we present new ⁸⁷Sr/⁸⁶Sr, ¹⁴³Nd/¹⁴⁴Nd, ²⁰⁶Pb/²⁰⁴Pb, ²⁰⁷Pb/²⁰⁴Pb, ²⁰⁸Pb/²⁰⁴Pb and δ¹⁸О isotopic data on 40 samples of the Thera pyroclastics. We also include some measurements of hydrogen isotopes. Methods of geochemical and isotopic analysis are described in Appendix 1. This chapter also presents some quantitative models of fractional crystallization and assimilation of crustal rocks. The geochemical data and models point towards the importance of crystal fractionation, magma mixing and assimilation of continental crust in magma genesis at Santorini. The chapter also documents temporal changes in geochemical features of Santorini magmas.