In this study, two bimaterial joining systems, namely, titanium coated glass/polyimide (TiGPI) and titanium/polyimide (TiPI) are considered. The joints were prepared by employing transmission type laser-joining procedure. Both the TiGPI and TiPI bimaterial systems were subjected to tensile loading using a microtester, and failure loads per unit bond length were documented. The average failure strengths of the TiPI and TiGPI samples were found to be 5.1 and 7.3 N/mm, respectively. It is thus clear from the failure data that the TiGPI joints are stronger (1.4 times) than the TiPI joints although same chemical bonds between titanium and polyimide (PI) exist for both the systems. It is thus believed that material surface morphology has contributed to such variation in the microjoint strengths. Later, atomic force microscopy (AFM) of titanium surfaces of both titanium coated glass and titanium foil was performed, and was observed that they had root mean squared (RMS) surface roughnesses of 220 and 55 nm, respectively. The surface roughness provides improved surface contact area, number of chemical bonds, and mechanical interlocking that may have resulted in higher bond strength for the TiGPI system.