Quicklime, rich in CaO(s), is generated by calcining limestone at high temperatures. Parallel-flow regenerative lime kilns are the most energy-effective industrial method available today. To prevent major disruptions in such kilns, a high raw material quality is necessary. Under some conditions, impurity-enriched material may adhere to limestone pebbles and enter the kiln. In this study, limestone and corresponding quicklime were analyzed to evaluate the extent and composition of surface impurities and assess the effect on quicklime product quality, here defined as free CaO. This was performed by sampling and analyzing limestone, quarry clay, laboratory-produced quicklime, and industrially produced quicklime with XRF, SEM/EDX, and XRD; interpretations were supported by thermodynamic equilibrium calculations. In the laboratory-produced quicklime, the surface impurities reacted with calcium forming Larnite, Gehlenite, Åkermanite and Merwinite, reducing the quicklime quality. The results showed that the limestone surface layer comprised 1.2 wt.-% of the total mass but possessed 4 wt.-% of the total impurities. The effect on industrially produced quicklime quality was lower; this indicated that the limestone surface impurities were removed while the material moved through the kiln. Multicomponent chemical equilibrium calculations showed that the quarry clay was expected to be fully melted at 1170 °C, possibly leading to operational problems.