The Gilbert damping of ferromagnetic materials is arguably the most important but least understood phenomenological parameter that dictates real-time magnetization dynamics. Understanding the physical origin of the Gilbert damping is highly relevant to developing future fast switching spintronics devices such as magnetic sensors and magnetic random access memory. Here, we report an experimental study of temperature-dependent Gilbert damping in permalloy (Py) thin films of varying thicknesses by ferromagnetic resonance. From the thickness dependence, two independent contributions to the Gilbert damping are identified, namely bulk damping and surface damping. Of particular interest, bulk damping decreases monotonically as the temperature decreases, while surface damping shows an enhancement peak at the temperature of ∼50 K. These results provide an important insight to the physical origin of the Gilbert damping in ultrathin magnetic films.