The ~50 or 570 ka old Lonar crater, India, was excavated in the Deccan Trap flood basalt of Cretaceous age by the impact of a chondritic asteroid. The impact-spherules known from within the ejecta around this crater are of three types namely aerodynamically shaped sub-mm and mm size spherules, and a sub-mm sized variety of spherule, described as mantled lapilli, having a core consisting of ash-sized grains, shocked basalt and solidified melts surrounded by a rim of ash-sized materials. Although, information is now available on the bulk composition of the sub-mm sized spherules (Misra et al. in Meteorit Planet Sci 7:1001–1018, 2009), almost no idea exists on the latter two varieties. Here, we presented the microprobe data on major oxides and a few trace elements (e.g. Cr, Ni, Cu, Zn) of mm-sized impact spherules in unravelling their petrogenetic evolution. The mm-sized spherules are characterised by homogeneous glassy interior with vesicular margin in contrast to an overall smooth and glassy-texture of the sub-mm sized spherules. Undigested micro-xenocrysts of mainly plagioclase, magnetite and rare clinopyroxene of the target basalt are present only at the marginal parts of the mm-sized spherules. The minor relative enrichment of SiO2 (~3.5 wt% in average) and absence of schlieren structure in these spherules suggest relatively high viscosity of the parent melt droplets of these spherules in comparison to their sub-mm sized counterpart. Chemically homogeneous mm-sized spherule and impact-melt bomb share similar bulk chemical and trace element compositions and show no enrichment in impactor components. The general depletion of Na2O within all the Lonar impactites was resulted due to impact-induced volatilisation effect, and it indicates the solidification temperature of the Lonar impactites close to 1,100 °C. The systematic geochemical variation within the mm-sized spherules (Mg# ~0.38–0.43) could be attributed to various level of mixing between plagioclase-dominated impact melts and ultrafine pyroxene and/or titanomagnetite produced from the target basalt due to impact. Predominance of schlieren and impactor components (mainly Cr, Ni), and nearly absence of vesicles in the sub-mm sized spherules plausibly suggest that these quenched liquid droplets could have produced from the impactor-rich, hotter (~1,100 °C or more) central part of the plume, whereas the morpho-chemistry of the mm-sized spherules induces their formation from the relatively cool outer part of the same impact plume.