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The extruded cordierite honeycomb structure from a stoichiometric formulation of talc, kaolinite, and alumina was subjected to TGA-DSC, dilatometric and XRD investigations. The experimental observations were made to identify the phase transformation sequence in order to understand the solid state reactions involved in the cordierite formation. A maximum cordierite content of 90% was achieved for the samples sintered at 1693 K with a soaking time of 4 h, corresponding to a lowest coefficient of thermal expansion (CTE) of 0.74 × 10−6/K (along the direction of extrusion) was observed. Attempts were made to establish correlations with cordierite content, processing temperature and CTE of the samples. A few mechanisms are proposed to explain our observations. Attempts are also made to rationalize the low CTE observed along the direction of extrusion on the basis of orientation of anisotropic cordierite crystals as revealed by the transverse I-ratio calculated from the XRD patterns. Effect of CaO doping on CTE of cordierite has been studied in the present work. It was observed that though there is an increase in bulk thermal expansion of cordierite honeycombs on CaO doping due to the absence of micro-cracks as reveled by thermal cycling hysteresis, axial anisotropy was found to be reduced significantly.