This dataset comprises geological field observations, whole-rock geochemical data (ICP-MS) and mineralogical data (XRD, SEM-EDS) for rock samples collected in and around the Kamativi area of Zimbabwe in October 2018. Samples of between 5 and 10 kilograms were collected in the field by a team of British Geological Survey (BGS) geologists. A set of polished thin sections was prepared at the BGS for mineralogical analysis undertaken by experienced analysts using SEM-EDS. A subset of samples was prepared at the BGS for whole-rock geochemical analysis by crushing and milling, the milled powders were sent to an accredited commercial laboratory in Canada for acid digestion and ICP-AES and ICP-MS analysis. A subsample of the powder was used for qualitative XRD analysis at the British Geological Survey. The data were collected to answer a research question about the ‘internal evolution of lithium pegmatites’ and how the mineralogy changes during cooling (i.e. crystallisation). Further details of the work can be found in READ_ME_information_about_analytical_methods_for_Kamativi_Zimbabwe.txt and in Shaw et al. (2022) - https://doi.org/10.3749/canmin.2100032