heat-dissipation structures, such as fins and micro/nanochannels, have been designed to efficiently dissipate heat from heat sources. [4][5][6] However, the inevitable gap between the heat source and heat exchanger results in thermal contact resistance (R c ), deteriorating heat dissipation performance. [7,8] The R c can be decreased by filling the gap with a thermal interface material (TIM). [1,7] A variety of different TIMs are available including thermal greases, adhesives, solders, and pads. [9] The pad-type TIM is a pre-formed thermally conductive film which can be compressed between the heat source and heat sink. This is removable which is advantageous for future disassembly and reassembly of the heat sink.The TIM can be classified based on directionality. [10] An anisotropic TIM, such as a graphite sheet, provides a high thermal conductivity (κ) in the aligned direction (≈1500 W m −1 K −1 ), but the κ in the perpendicular direction is significantly lower (≈5 W m −1 K −1 ). [11] Directional heat manipulation has been actively investigated using aligned hexagonal boron nitride platelets, [12] thermal metamaterials, [13,14] and aperiodic superlattice structures. [15,16] These technologies have potential applications in anisotropic TIMs. An isotropic TIM provides a uniform κ in all directions and can be synthesized by dispersing randomly-oriented thermally conductive fillers in a polymer matrix. [10,17,18] The κ of commercial isotropic TIMs is typically small (≈10 W m −1 K −1 ). Various types of fillers, such as carbon nanotubes, graphene, boron nitrides, metal nanoparticles (NPs), and ceramic particles, have been actively investigated to enhance κ. [10,17,[19][20][21][22] Polyurethane, epoxy (EP), and silicone rubber have been employed as a matrix to achieve high compressibility and conformability. [10,17,19,23] In this study, pad-type isotropic polymeric TIMs are primarily analyzed.Another important parameter of TIMs, in addition to κ, is thermal resistance. [24] The total thermal resistance (R t ) is composed of the specimen thermal resistance (R s = l/κ, l = specimen thickness) and R c . In order to decrease R s , the κ of TIMs can be increased by increasing filler concentration. However, the high filler concentration also increases elastic modulus (E), or decreases softness, making the conformal contact with a matingThe ORCID identification number(s) for the author(s) of this article can be found under