A thermal interface material (TIM) includes a modified release layer having an organosilane-coated surface covalently bound to a TIM formulation layer. The modified release layer may be formed by applying an organosilane (e.g., vinyltriethoxysilane) to the surface of a thermally conductive release layer (e.g., aluminum foil). The organosilane reacts with hydroxyl groups on the surface of the thermally conductive release layer. The TIM formulation layer may be formed by applying a TIM formulation (e.g., a graphite TIM formulation) containing an unsaturated monomer (e.g., methyl acrylate) to the organosilane-coated surface of the modified release layer, and then curing the TIM formulation so that the unsaturated monomer of the TIM formulation reacts with the organosilane-coated surface of the modified release layer.