The mechanical response of syntactic foams comprising hollow thermoplastic microspheres (HTMs) embedded in a polyurethane matrix were experimentally examined under uniaxial compressive strain. Phenomenological strain energy models were subsequently developed to capture both the axial stress-strain and transverse strain response of the foams. HTM syntactic foams were found to exhibit increased small-strain stiffness with reduced density, revealing a highly tuneable and extremely lightweight syntactic foam blend for applications. The foams were also found to become strongly compressible at large strains and possess a high threshold for plastic deformation, making them a robust alternative to hollow glass microsphere syntactic foams. The non-standard transverse strain relationship exhibited by HTM syntactic foams at high filling fractions was captured by Ogden-type strain energy models. The thermal characteristics of these syntactic foams were also explored with Differential Scanning Calorimetry testing which showed that HTMs have a negligible impact on the thermal characteristics of the matrix.