This thesis focuses on establishing the scientific and engineering foundations for gaining a fundamental understanding of the mechanisms and critical parameters governing the processing of integral-skin low-density polyolefin foams in rotational foam molding. The presented research is particularly intended to broaden the knowledge in the field of manufacturing adjacent, but clearly distinct, layers of non-cellular and cellular structures, consisting of identical or compatible plastic grades, using a single-charge processing concept. Although this technology is beneficial for the efficacy of the molding process and the structural homogeneity of the moldings, its optimization raised a fairly large number of fundamental issues that had to be resolved through further research. In this context, an attempt has been made to establish rigorous, experimentally validated, theoretical models that describe the phenomena identified as the fundamental challenges of this technology. The major contributions of this thesis include:​ (i) optimization of the single-charge rotational foam molding process for the manufacture of both PE/PE and PE/PP integral-skin cellular composites, (ii) development of a two-step oven temperature profile that prevents the foamable resins invading the solid skin layer and ensures that skin formation always completes prior to the activation of the foamable resin, (111) fundamental study of the adherence behavior of powders and foamable pellets to a hightemperature rotating mold wall, (iv) fundamental study of the lifespan of CBA-blown bubbles in non-pressurized non-isothermal polymer melts using hot-stage optical microscopy and digital imaging, (v) development of a detailed theoretical model involving diffusion, surface tension, and viscosity to simulate the observed foaming mechanism, and (vi) fundamental study of the rotofoamablility of polyolefin resins using both dry blending and melt compounding based methods and characterization of rheological and thermal properties.