In the present investigation, dissimilar materials such as electrolytic tough pitch copper, and aluminum 6061-T651 were welded by friction stir welding technology. Effects of tool tilt angle on the mechanical and metallurgical properties were studied experimentally for dissimilar material systems. In the present study, the tool tilt angle was varied from 0° to 4° with an interval of 1°, while the other parameters such as rotational speed, welding speed, tool pin offset, and workpiece material position were kept constant. Macrostructure analysis, tensile test, macro hardness measurement, scanning electron microscopy, and energy dispersive x-ray spectrographic tests were performed to evaluate the weld properties of dissimilar copper-aluminum joints. The results revealed that a defect free dissimilar copper-aluminum friction stir welding was achieved by tilt angles 2°, 3°, and 4°. The maximum tensile strength was reported to be 117 MPa and the macro hardness was reported to be 181 VH (in the nugget zone) at a tilt angle of 4°. The macro hardness was increased as the tilt angle increases from 0° to 4°. In addition to this, the thermo-mechanically affected zone (at the copper side) was found to be the weakest zone for a dissimilar copper-aluminum friction stir welding system.