The combined capacity of Jute Fibers (JF), the reinforcement, and Ground-Granulated Blast-Furnace Slag (GBFS), the binder, was examined as a sustainable solution towards ameliorating the inferior engineering properties of micaceous clays. A total of sixteen JF + GBFS mix designs, i.e., JF (% by total mass) = {0, 0.5, 1.0, 1.5} and GBFS (% by total mass) = {0, 3, 6, 9}, were tested for unconfined compression (UC) strength; for those mix designs containing GBFS, curing was allowed for 7 and 28 days prior to testing. Scanning electron microscopy (SEM) studies were also carried out to observe the evolution of fabric in response to JF, GBFS and JF + GBFS amendments. The greater the JF content the higher the developed strength and stiffness up to 1% JF, beyond of which the effect of JF-reinforcement led to some adverse results. The JF inclusions, however, consistently improved the ductility and toughness of the composite. The addition of GBFS to the JF-reinforced samples improved the soil–fiber connection interface, and thus led to further improvements in the composite’s strength, stiffness and toughness. The mix design “1% JF + 9% GBFS” managed to satisfy ASTM’s strength criterion and hence was deemed as the optimum choice in this investigation. Finally, a non-linear, multivariable regression model was developed and validated to quantify the peak UC strength as a function of the composite’s index properties. The proposed model contained a limited number of fitting parameters, all of which can be calibrated by little experimental effort, and thus implemented for preliminary design assessments.