Recently, plasmonic nanofluids (i.e., a suspension of plasmonic nanoparticles in a base fluid) have been widely employed in direct-absorption solar collectors because the localized surface plasmon supported by plasmonic nanoparticles can greatly improve the direct solar thermal conversion performance. Considering that the surface plasmon resonance frequency of metallic nanoparticles, such as gold, silver, and aluminum, is usually located in the ultraviolet to visible range, the absorption coefficient of a plasmonic nanofluid must be spectrally tuned for full utilization of the solar radiation in a broad spectrum. In the present study, a modern design process in the form of a genetic algorithm (GA) is applied to the tailoring of the spectral absorption coefficient of a plasmonic nanofluid. To do this, the major components of a conventional GA, such as the gene description, fitness function for the evaluation, crossover, and mutation function, are modified to be suitable for the inverse problem of tailoring the spectral absorption coefficient of a plasmonic nanofluid. By applying the customized GA, we obtained an optimal combination for a blended nanofluid with the desired spectral distribution of the absorption coefficient, specifically a uniform distribution, solar-spectrum-like distribution, and a step-function-like distribution. The resulting absorption coefficient of the designed plasmonic nanofluid is in good agreement with the prescribed spectral distribution within about 10% to 20% of error when six types of nanoparticles are blended. Finally, we also investigate how the inhomogeneous broadening effect caused by the fabrication uncertainty of the nanoparticles changes their optimal combination.