Encapsulant is one determining factor underpinning the device lifetimes of organic optoelectronics. However, encapsulant seriously needs improvement in optical, thermal, and mechanical properties, especially to develop organic light emitting diodes. In this study, we prepared an in situ crosslinked organosilane composite containing benzyloxy and glycidyl-modified quartz microcrystal (mQMC) as high performance encapsulant. In the present work, methylphenylsilanediol (MPSD) was introduced as a novel crosslinker to impart appropriate structural strength. Along with increasing mQMC fillers, this organosilane system shows improved properties, such as refractive index, thermal stability, and storage modulus. Specifically, these hybridized mQMCs in the organosilane framework may facilitate an approximate two-fold increase (0.238 W/(m·K)) in overall thermal conductivity at the determined concentration.