Carbon nanomaterials are an emerging class of nano-reinforcements to substitute for metal-based nanomaterials in polymer matrices. These metal-free nano-reinforcement materials exhibit a high surface area, thermal stability, and a sustainable nature. Compared to conventional reinforcements, nano-carbon-reinforced polymer composites provide enhanced mechanical and thermal properties. While previous reviews summarized the functionality of nanocomposites, here, we focus on the thermomechanical properties of nano-carbon-reinforced nanocomposites. The role of carbon nanomaterials, including graphene, MXenes, carbon nanotubes, carbon black, carbon quantum dots, fullerene, and metal–organic frameworks, in polymer matrices for the enhancement of thermal and mechanical properties are discussed. Different from metal-based nanomaterials, carbon nanomaterials offer high specific strength, abundance, and sustainability, which are of considerable importance for commercial-scale applications.