Proppant particulates are commonly used in hydraulic fracturing operations to maintain one or more fractures in an opened state following the release of hydraulic pressure. In complex fracture networks, it can be difficult to deposit proppant particulates fully within the fractures. In addition, low crush strengths may result in problematic fines formation. Polyaromatic hydrocarbons, commonly encountered in various refinery process streams, may serve as an advantageous precursor to proppant particulates. Polyaromatic hydrocarbons may undergo crosslinking under acid-catalyzed conditions in an aqueous solvent in the presence of a surfactant to form substantially spherical particulates that may serve as effective proppant particulates during fracturing operations. In situ formation of the proppant particulates may take place in some cases.