The design of new composites based on a polypropylene (PP) matrix and filler fly ash particles leads to changes in processability, morphology, and physical properties of the raw thermoplastic. The new materials should combine the processability of common thermoplastics with improved toughness. We have designed more environmentally friendly composites filled with residual ash. To improve composite toughness (one of the principal drawbacks of these PP/ash composites), a new olefin block copolymer (OBC) was included in the filler-matrix interface, and to modify the ash surface, an organosilane was used to enhance interface strength. The present work analyzes the influence of composite formulation on the morphological, mechanical, and rheological properties of the new composites. In terms of rheological properties, modulus and viscosity were enhanced as a function of the amount of filler added. The incorporation of a silane coupling agent into composites brought about beneficial changes in morphology and rheology, related with improved dispersion of ash particles and increased filler-matrix interactions. Finally, when OBC was added to the filler-matrix interface, composite morphology was more homogenous. The best rheological and mechanical properties were obtained when the ratio of OBC to fly ash particles was 1:2.