Accurate small animal surface reconstruction is important for full angle non-contact fluorescence molecular tomography (FMT) systems. In this letter, an optimal surface reconstruction method for FMT is proposed. The proposed method uses a line search method to minimize the mismatch between the reconstructed three-dimensional (3D) surface and the projected object silhouette at different angles. The results show that the mean mismatches of the 3D surfaces generated on three live anesthetized mice are all less than two charge coupled device (CCD) pixels (0.154 mm). With the accurately reconstructed 3D surface, in-vivo FMT is also performed.