Nanocomposites with exfoliated 2D materials are highly sought after due to resulting material enhancement of barrier and increased modulus among others. In the past, this was achieved by using polyols that were effective but caused a significant drop in the glass transition temperature of the nanocomposite. In this contribution, alpha-zirconium phosphate (ZrP) nanoplatelets were covalently modified to allow for dispersion in solvents with varying hydrophobicity and poly(methyl methacrylate) (PMMA) for the first time. The nanoplatelets were prepared by using a polyetheramine surfactant to achieve exfoliation, followed by modification with epoxides. Combinations of different epoxides were shown capable of tuning the functionality and hydrophobicity of the exfoliated ZrP in organic media. After grafting glycidyl methacrylate and cyclohexene oxide to the surface of ZrP, an in situ free radical polymerization of MMA allowed for high concentrations of self-assembled exfoliated ZrP in a PMMA matrix.