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Angle-resolved core-level photoemission has been utilized to study the surfaces of crystalline thin films of manganite La1-xCaxMnO3 (x=0.1 and 0.35). It is found that both the surface termination and Ca surface concentration depend on the bulk Ca concentration. For La0.65Ca0.35MnO3, the terminal layer is predominately Mn-O, while for La0.9Ca0.1MnO3, the majority of the surface is La/Ca-O terminated. Both surfaces exhibit a large enhancement in the Ca concentration compared to the bulk with the La0.9Ca0.1MnO3 sample, having a larger surface Ca concentration than for the La0.65Ca0.35MnO3 material.