During the last two decades, considerable interest has been expressed in the development of lime and lime plaster products in the Near Eastern Pre‐Pottery Neolithic B. The occurrences of lime products in numerous Levantine sites have raised questions concerning their methods of production, their role in the development of craft specialization, and their social and economic implications. Lime plaster was the first product that entailed the intentional chemical alteration of materials and the complete control over their properties. This was probably the reason for the wide spectrum of uses to which it was put, amongst which “daily” architectural functions appear to coexist with the symbolic or spiritual applications of this material. Amongst the variety of plaster products which appeared in the PPNB, it seems that the practice of skull plastering and sculpture production was the most “socially oriented” one, lacking any apparent relation to daily, functional use. In the present study two modeled skulls and a collection of plaster sculptures from Jericho were examined by means of thin section petrographic analysis, inductively coupled plasma atomic emission spectrometry, scanning electron microscopy, X‐ray diffraction, and Fourier‐transform infrared spectrometry. The results of the mineralogical and chemical analyses, when compared to data obtained from similar artifacts from other sites, demonstrate pronounced intersite variability in the methods of production of the skull and sculpture modeling. The full implications of this issue are discussed in detail in the paper.