To maintain acceptable device temperatures in the new generation of electronic devices under development for high-power applications, conventional liquid cooling schemes will likely be superseded by multi-phase cooling solutions to provide substantial enhancement to the cooling capability. The central theme of the current work is to investigate the two-phase thermal performance of carbon-based nanostructured coatings in passive and pumped liquid-vapor phase-change cooling schemes. Quantification of the critical parameters that influence thermal performance of the carbon nanostructured boiling surfaces presented herein will lead to improved understanding of the underlying evaporative and boiling mechanisms in such surfaces. A flow boiling experimental facility is developed to generate consistent and accurate heat transfer performance curves with degassed and deionized water as the working fluid. New means of boiling heat transfer enhancement by altering surface characteristics such as surface energy and wettability through light-surface interactions is explored in this work. In this regard, carbon nanotube (CNT) coatings are exposed to low-intensity irradiation emitted from a light emitting diode and the subcooled flow boiling performance is compared against a non-irradiated CNT-coated copper surface. A considerable reduction in surface superheat and enhancement in average heat transfer coefficient is observed. In another work involving CNTs, the thermal performance of CNT-integrated sintered wick structures is evaluated in a passively cooled vapor chamber. A physical vapor deposition process is used to coat the CNTs with varying thicknesses of copper to promote surface wetting with the working fluid, water. Thermal performance of the bare sintered copper powder sample and the copper-functionalized CNT-coated sintered copper powder wick samples is compared using an experimental facility that simulates the capillary fluid feeding conditions of a vapor chamber. Nanostructured samples having a thicker copper coating provided a considerable increase in dryout heat flux while maintaining lower surface superheat temperatures compared to a bare sintered powder sample; this enhancement is attributed primarily to the improved surface wettability. Dynamic contact angle measurements are conducted to quantitatively compare the surface wetting trends for varying copper coating thicknesses and confirm the increase in hydrophilicity with increasing coating thickness. The second and relatively new carbon nanostructured coating, carbon nanotubes decorated with graphitic nanopetals, are used as a template to manufacture boiling surfaces with heterogeneous wettability. Heat transfer surfaces with parallel alternating superhydrophobic and superhydrophilic stripes are fabricated by a combination of oxygen plasma treatment, Teflon coating and shadow masking. Such composite wetting surfaces exhibit enhanced flow-boiling performance compared to homogeneous wetting surfaces. Flow visualization studies elucidate the physical differences in nucleate boiling mechanisms between the different heterogeneous wetting surfaces. The third and the final carbon nanomaterial, graphene, is examined as an oxidation barrier coating for liquid and liquid-vapor phase-change cooling systems. Forced convection heat transfer experiments on bare and graphene-coated copper surfaces reveal nearly identical liquid-phase and two-phase thermal performance for the two surfaces. Surface analysis after thermal testing indicates significant oxide formation on the entire surface of the bare copper substrate; however, oxidation is observed only along the grain boundaries of the graphene-coated substrate. Results suggest that few-layer graphene can act as a protective layer even under vigorous flow boiling conditions, indicating a broad application space of few-layer graphene as an ultra-thin oxidation barrier coating