Hybrid phenol-formaldehyde (PF) resins represent one of the most important niche groups of binding systems for composites. New industrial needs, environmental requirements, and price fluctuations have led to further research on materials with enhanced mechanical and thermal properties. The preparation of novel hybrid materials can be achieved by inclusion of various elements or functional groups in the organic polymer phenolic framework. Herein, we report the synthesis and characterization of a PF-based hybrid material with different nanoscale silicone species and ZnAl-layered double hydroxide (LDH). The main goals of this study were to improve the synthetic pathways of hybrid resin, as well as to prepare granulated composite materials and test samples and determine their characterization. Added inorganic species increased the glass-transition temperature by a minimum of 8 °C, which was determined using differential scanning calorimetry (DSC). Rheological properties (melting viscosity and flow distance) of the hybrid resin were measured. The homogeneity of distribution of added species across the organic matrix was evaluated with scanning electron microscopy (SEM). With synthesized new hybrid-binding systems, we prepared different granulated composite materials and evaluated them with the measurements of rheological properties (flow curing characteristics). Tensile strength of samples, prepared from granulated composite material, improved by more than 5%.