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One type of multimodal (comprised of nanometer and sub-micrometer WC particles) and two types of conventional (comprised of nanometer and sub-micrometer WC particles, respectively) WC/Co powders were deposited on AISI 304L stainless steel substrates by using high velocity oxygen fuel spraying. The use of multimodal WC particles was indicated to have a beneficial effect on the solar absorptance (α) of the WC/Co coatings. The α of the multimodal WC coating reached 0.87, which was much higher than what can be achieved by either fine (0.82) or coarse powders (0.80) alone. By microstructural analysis, the enhancement in solar absorptance of the multimodal WC/Co coating was ascribed to the layer of distributed WC particles. During the thermal spraying, the nanostructured WC particles underwent rapid melting for the large specific surface area while the aggregated powders were heated, but not necessarily melted. The molten nano-WC would fill the available pores between the softened and heated aggregates, providing a layered distribution of WC particles for the spray-deposited coating. In this condition, the light-trapping in the multimodal coating will be enhanced due to the efficient light reflection among the multimodal WC particles, which contributes to the enhancement of solar absorptance.