This study investigates the development of novel montmorillonite/castor oil blends to formulate sustainable lubricating greases to promote the replacement of petrochemicals industry-derived materials by substances obtained from renewable sources. Specifically, the effect of the thickener concentration on the rheological, chemical, thermal, tribological properties, and atomic force microscopy (AFM) microstructure of these systems were studied. The results showed that the C20A nanoclay content could be used to modulate the viscosity values, the linear viscoelastic functions, and tribological properties of these montmorillonite dispersions. In general, these gel-like dispersions exhibited remarkable lubricant properties; the samples showed values of the friction coefficient and wear scars similar or lower than those obtained with model bentonite grease.