A method to blend starches and polyethylene, and thus improve the environmental footprint, was investigated. Unlike traditional methods that utilize compatibilizers or rely on reactive extrusion to achieve the desired material compatibility, a high amylose starch, such as Gelose 80, was mixed with native starch, converted to thermoplastic starch, and compounded with Ecoflex and polyethylene. Films showed good integrity and were evaluated for mechanical properties, anaerobic biodegradability, and structure changes both before and after anaerobic sludge digestion. Mechanical properties were sufficient that these films might be utilized in a number of applications but were not recommended as a sustainable solution. Biodegradation was below the theoretical maximum, was not a linear function of the amount of biodegradable materials incorporated in the films, and was depressed further as the proportion of polyethylene increased due to an encapsulation effect. Structural evaluation showed the components of the blends remained as separate phases and the structure of the Gelose 80 was reminiscent of interphase material. Biodegradation yield appeared to be principally driven by connectivity of the starches within the films to the anaerobic sludge digestion environment. Recommendations for additional studies were given. (C) 2010 Wiley Periodicals, Inc. J Appl Polym Sci 120: 1808-1816, 2011