Polymer composites with high dielectric constant and low loss tangent are highly regarded as substrates for modern high-speed electronics. In this work, we analyze the high-frequency dielectric properties of two types of composites based on polypropylene infused with high-dielectric-constant microparticles. Two types of fillers are used: commercial ceramics or titanium oxide (TiO2) with different concentrations. The key observation is that adding the fillers causes an increase of dielectric constants by around 100% (for highest loading) up to 4.2 and 3.4, for micro-ceramics and TiO2 based composites, respectively. Interestingly, for the TiO2 composite, the loss tangent depends on the filler loading volume, whereas the other composite has a slightly increasing tendency, however, being at the level ~ 10–3. To explain the experimental results, a theoretical model determined by microwave reflection and transmission through a representative volume element is proposed, which allows the investigation of the impact of volume ratio, grain shape, aggregation, and size on the loss tangent and permittivity evolution. This approach could be used for modeling other low dielectric loss materials with inclusions.