Investigating the design space available in nanofilled polymers is expected to produce materials with unique structure-property relationships. In this work, the concept of tensegrity is used as inspiration for microstructural design. Tensegrity is an elegant and efficient structural design, relying upon interactions between elements, specifically elements in compression which are connected through a tensioned web. In this embodiment, the nanoparticles are considered the compressive elements, and the polymer matrix, when suitably processed, is considered the tensioned web. Nanocomposite materials containing polymer-decorated hydroxyapatite nanoparticles were used to evaluate the tensegrity-inspired approach. Nanocomposite systems with a semi-crystalline matrix (polyethylene oxide) and an amorphous matrix (polymethyl methacrylate) were prepared and characterized with compatible polymer decorated nanoparticles. The results showed that the nanocomposite with a semi-crystalline matrix was more promising as a candidate for producing the tensegrity-inspired microstructure and that the concept could produce improved thermomechanical properties in the glassy temperature regime. (C) 2017 Elsevier Ltd. All rights reserved.