A precision adiabatic calorimeter has been used to determine the free energy of formation of polyethylene single crystals, grown at 70 and 9O"C, in the range 30-80°C. When the temperature is higher than about 10°C above the growth temperature the crystals slowly release heat and equilibrium conditions can no longer be attained (in a time of 1-2 days). The annealing process responsible for the heat release is discussed. Surface free energies have been calculated using both the Keller and Flory models to represent the surface morphology of the crystal. The assumption of regular chain folding leads to the more reasonable results. A two-fold decrease of surface free energy is found as the temperature is changed from 30 to 80°C; it is suggested that this is due to a progressive loosening of the sharp chain folds. The heat of fusion, 285 J g-1, found for the fully extended, infinite crystal is in excellent agreement with previous results involving different techniques.