In this study, an experimental investigation was conducted on the dynamics and heat-transfer characteristics of liquid film flow for upward- and vertical-facing spray cooling. The heat-transfer performances at different inlet pressures, nozzle-to-surface distances, and heat flux inputs between the two orientations were compared, and the morphologies, wetted areas, and velocities of the isolated liquid films were quantitatively captured. The morphologies of the HFE-7100 liquid films and their distributions on the vertical and upward surfaces exhibited no significant differences. In most cases, the heat-transfer performance of the upward surface was slightly better than that of the vertical surface. Gravity affected the velocity of the isolated liquid films on a smooth vertical surface, whereas its effect was significantly suppressed on an unpolished surface. The Bond number of the isolated liquid film flow on the upward surface was verified to be naturally smaller than that on the vertical surface. Dimensionless groups, including the Bo, We, and Re numbers of the liquid film flow in spray cooling, were obtained to further account for the effect of gravity. The reason why the dimensionless groups presented such small orders was explained. The data map of liquid film flow (dimensionless groups) during spray cooling was further enriched.