In the present work, the effects of laser surfacing aiming at modifying the surface roughness on NiTi sheets prior to the application of ultrasonic welding (USW) were investigated. Three different configurations joining original and laser surfaced specimens were performed: original/original (referred as O/O), original/treated (referred as O/T), and treated/treated (referred as T/T). The influence of surface roughness on the interface formation, diffusion, and mechanical properties was investigated. It is observed that when both bonding surfaces becomes rougher (T/T configuration), the joint strength is the highest, followed by both smooth bonding surfaces (O/O configuration), and the strength of the joint is the lowest when only one of the bonding surfaces was roughened (O/T configuration), which is related to the degree of plastic deformation at the joining interface. The main joining mechanism of NiTi to the Al interlayer was a metallic bonding caused by shear plastic deformation and formation and growth of micro welds at the joining interfaces. Laser surfacing facilitates the metallic bonding, which is directly reflected in the change of the thickness of the Al interlayer after USW. This also helps to produce a mechanical interlocking at the interface, although there is no significant difference in the elemental diffusion. Interfacial failure occurred in all joints tested under different surface contact conditions and exhibited ductile-like fracture characteristics.