In order to develop a numerical simulation model of the high-speed twin-roll casting (HSTRC) process, an appropriate melt/strip heat transfer coefficient (HTC) is required. In the present study, the strip temperature was directly measured by using the traveling thermocouple technique. Then, we tried to determine the reasonable HTC values, which conformed well with the temperature curves obtained experimentally. The results showed that the HTC values increased with increasing casting speed. Moreover, the overall HTCs were much higher than those reported so far. We believe that a large hydrostatic pressure, induced by a high melt pool level, and a sufficient roll separating force helped improve the contact condition between the solidifying shell and the roll surface.