This study fundamentally examines the characteristics of solidification cracking in Cu-Al5052 single-mode fiber laser welding by utilizing uncoated and Ni-P coated Cu plates for the high durability busbar welding of pouch-type lithium-ion battery packs. Weld solidification cracking was confirmed regardless of Ni-P coating for both weld materials. However, there were differences in the regions of crack occurrence. Unlike the uncoated Cu-Al5052 welds where cracks occurred randomly within the fusion zone, for the Ni-P coated Cu-Al5052 welds, solidification cracks were concentrated near the faying surface of the upper and lower materials, particularly near the fusion line. The effect of the Ni and P components on the solidification cracking susceptibility, i.e., the welding solidification temperature range, was considered. Diffusion-controlled Scheil’s solidification calculations revealed that the mushy zone range enlarged with the use of a Ni coating layer. It was confirmed that an extremely wide mushy zone range of 1060 K was calculated at the solidification cracking region. Furthermore, P was also identified as an element that expands the solidification temperature range based on the Cu-P binary system. Consequently, during the laser welding of Cu-Al5052 dissimilar materials, the behavior of solidification cracking in the welds is influenced by the composition of the coating material and the incorporated composition within the weld fusion zone. Hence, it is necessary to select the optimal coating material and layer thickness considering weld solidification cracking susceptibility.