Particulate composites are found in a wide range of applications. Their heterogeneous microstructure affects their bulk behavior and structural performance, however tools for predicting this important structure-property relationship are still lacking. In this study, a numerical method that can provide predictions of the mechanical response of a particulate polymeric matrix composite as a function of volume fraction and particle mean diameter is presented. The work is derived for an alumina trihydrate filled poly(methyl methacrylate) but the methodology is generic and can be used for any particulate composite. Representative Volume elements are determined through images obtained from scanning electron microscopy. The model takes into account the possibility of failure through interface debonding as well as cracks through the matrix. The model predictions for the modulus and fracture strength of the composites are validated through independent experiments on the composite. The numerical results are also used to qualitatively explain the trends measured regarding the fracture toughness of the composites. Compared to other literature on particulate composites, our study is the first to report accurate stress–strain distributions as well as fracture predictions whilst all the necessary model parameters defining the failure criteria are all derived through independent experiments. This paves the way for a relatively simple methodology for determining structure-property relationships in composites design, enabling smarter material utilization and optimal mechanical properties.