The use of different stereospecific metallocene catalysts: isotactic (iPP, C2-symmetry) and syndiotactic (sPP, Cs-symmetry) has been investigated in order to improve the mechanical properties of polypropylene/nanoclay nanocomposites obtained by in-situ polymerisation. Stereoregular nanocomposites have been synthetized in the presence of polar comonomers (1-undecenol (R-OH) and acid-undecenoic (R-COOH) for improving the matrix-nanoclay chemical compatibility. An important study of variables: amount of nanoparticles used as co-catalyst support, type of catalyst, type and amount of comonomer have been studied in a full factorial design of experiments in order to identify the main factors that achieve a balance between the stiffness and toughness of the polypropylene nanocomposites. Important results were found from ANOVA (analysis of variance): the nanoclay has a greater influence on the syndiotactic configuration and, the amount of polar comonomer is the main factor in maximising mechanical properties, irrespective of stereospecificity of the polypropylene nanocomposites.