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Using known parameters for the surface and interfacial tension, the work of adhesion of PMMA with PLA and styrenic polymers has been calculated. The results indicated that PMMA, an abundant and economical homopolymer, could serve as an effective compatibilizer, rivaling complex and costly block copolymers for PLA/styrenic blends. Blends of PLA with either SAN or ABS were produced with added 1%–10% PMMA. Tensile and impact toughness data show that the blends display properties comparable to those of PP with only 4% added PMMA. Deuterated-secondary ion mass spectrometry (DSIMS) performed with deuterated PMMA indicated that this corresponded to the formation of an interfacial layer approximately 2Rg thick, as the optimal thickness for integrating two polymers, without the formation of a third brittle layer. Blends with ABS showed an increase of nearly 300% in impact toughness compared to …