Preceramic polymer-grafted nanoparticles (PCPGNPs) are emerging as next-generation ceramic precursors due to their ability to form tunable networks, reduce shrinkage, and enhance ceramic yield. In this study, we examine PCPGNPs composed of silica nanoparticle cores grafted with poly(1,1-dimethylpropylsilane), suspended in the preceramic resin SMP-877. We investigate how low-temperature thermal treatments affect the rheological, structural, and dynamic behavior of these hybrid systems. Above 50–60 wt% PCPGNP, the system undergoes percolation, forming a space-spanning network with significantly enhanced modulus and viscosity. Rheology and X-ray photon correlation spectroscopy (XPCS) reveal that graft overlap and crosslinking lead to persistent jammed states, even upon cooling, correlating with improved ceramic yield. These insights offer critical design rules for processing high-performance preceramic materials, with implications for aerospace, heat shielding, and friction-resistant applications.
