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Stabilization of an amorphous solid against devitrification can be achieved using additives that interact specifically with the parent molecule, and restrain it from rearranging into a crystal lattice. The amorphous form of celecoxib (CEL) was stabilized by poly(vinylpyrrolidone) (PVP), both in the solid state and during dissolution. A comprehensive characterization of CEL−PVP binary amorphous systems by thermal, spectroscopic, and computer simulation techniques provided greater insight into the molecular interaction between the two species. PVP antiplasticized the amorphous CEL, thus raising its glass transition temperature (T_g) and restricting the molecular mobility. The T_gmix values for CEL−PVP binary amorphous systems of varying composition showed positive deviation from those predicted through the Gordon−Taylor/ Kelley−Bueche equation, thus indicating a molecular interaction between CEL and PVP …