Global industries strive towards the production of materials with superior mechanical characteristics, and their development remains a big challenges. One of the more interesting materials that exhibit these properties are silicate-filled epoxy molding compounds (EMCs). A good interaction between silicate filler and epoxy matrix is generally needed to achieve advantageous mechanical properties, as well as the desirable rheological behavior of EMCs. Understanding the influence of different organosilane coupling agents on the rheological and mechanical properties of EMCs is essential in the development and optimization of the manufacturing process. For this matter, a mixture of calcium silicate and aluminosilicate was treated by using organosilane coupling agents with different chemical structures and thus treated silicates were applied as fillers in the EMCs. The thermal behavior of the organosilane-modified, silicate-filled EMCs was studied by using differential scanning calorimetry (DSC) and thermomechanical analysis (TMA). Flow-curing behavior (torque rheometer) and spiral flow length measurement (EMMI) were used to monitor the rheological properties and reactivity of the EMCs. The results showed that 3-glycidyloxypropyltrimethoxysilane- and 3-aminopropyltriethoxysilane-treated filler had a greater influence on the tensile strength of hot-pressed test samples, while 3-aminopropyltriethoxysilane and a blend of primary and secondary aminosilanes had a more significant impact on the rheological behavior of the material.