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Novel compositions of methylcellulose in ethylene, propylene and butylene glycol were investigated for their thermal gel formation. These compositions have previously been found useful for inkjet-printing-based additive manufacturing processes as support materials. Experimental techniques such as viscosity measurements between 20 °C–150 °C–20 °C, differential scanning calorimetry (DSC) and X-ray diffraction (XRD) were used and the results showed that the gel formation upon cooling is caused by polymer–polymer association. The results also show that, for methylcellulose, propylene glycol is a better solvent than ethylene glycol and butylene glycol. Since no chemical reaction is involved, these gels can be used as support materials for jetting-based additive manufacturing processes.