The coefficient of thermal expansion (CTE) of hydrogenated amorphous carbon (a-C:H) was investigated as a function of the concentration of sp2 hybridization. The CTE, determined using the thermally induced bending technique, depends on the concentration of sp2 bonded carbon, increasing to the value of graphite as the sp2 concentration approaches 100%. By using a combination of the thermally induced bending technique and nanohardness measurements, we extract separately the Young’s modulus and Poisson’s ratio of the a-C:H films as function of the sp2 concentration.