Disclosed are exemplary embodiments of highly compliant non-silicone putties and thermal interface materials including the same. In an exemplary embodiment, a non-silicone putty includes at least one thermally-conductive filler and at least one other filler including hollow polymeric particles in a non-silicone polymer base or matrix. The non-silicone putty may have a thermal conductivity of at least about 3 Watts per meter-Kelvin and/or may have a hardness of less than about 30 Shore 00.