This study characterizes and compares coffee chaff (CC) and spent coffee grounds (SCG), the two most useful coffee waste products, and evaluates their performance as fillers and/or reinforcing agents in polymer composites. The morphologies of the CC and the SCG were studied using a scanning electron microscope (SEM). Detailed compositional and elemental analyses of the samples were carried out using several techniques. The thermal stabilities of the two types of biomass were evaluated using thermogravimetric analysis (TGA). Infrared spectroscopy was performed to investigate the functional groups available on the surface of the biomass. It was found that the CC had higher thermal stability, lower fat content, and a denser fibrous structure than the SCG, making it potentially a more suitable material than the SCG for use as a reinforcing filler in polymer composites. To verify this potential, CC and SCG filled polypropylene composites were produced and evaluated.