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  1. Developing an environmentally benign styrene foam is a critical environmental need. Supercritical CO2 use in foams has proven to be a valuable path. Adding fillers to increase bubble nucleation has been pursued concurrently. A prominent filler used is high surface area fillers, such as smectic clays. However, all studies to date show a limit of 152% in compressive moduli and 260% in the compressive stress. The values, even with such gains, limit structural application. A seminal work in 1987 by Suh and Cotton proved that carbonyl linkages in calcium carbonates and CO2 interact and impact nucleation efficiency and performance in supercritical CO2 foams. In this paper, a high surface area clay (layer double hydroxides) which begins in an exfoliated state, then functionalized with a long chain alkyl carboxylate (stearic acid) is synthesized. The result is a remarkable multi-fold improvement to the compressive properties in comparison to polystyrene (PS); a 268% and 512% increase in compressive modulus and strength, respectively. Using a pre-delaminated approach, the higher surface area was achieved in the clays. The presence of the stearate improved the interactions between the clay galleries and PS through hydrophobic-hydrophobic interactions. The glass transition temperature of the nanocomposites was observed to shiftmore »to higher values after foaming. The results point to a new path to increase performance using a pre-delaminated clay with functional groups for environmentally benign foams« less