Fly ash, a by-product of thermal power stations, was used as a filler in natural rubber (NR) in presence of 5-10 phr of phosphorylated cardanol prepolymer (PCP) and hexamethylene tetramine cured PCP (PCPHM). The compositions modified with the cardanol-based resins showed lower power consumption for mixing, lower cure time, improved tensile properties and tear strength, and higher thermal stability. Scanning electron microscopy of the fracture surfaces of the tensile-failed specimens showed finer and more uniformly distributed filler particles in the rubber matrix in the presence of PCP/PCPHM. The cardanol-based resins are expected to function as a coupling agent between the filler and rubber leading to the improvement in mechanical properties.