In this study, a new method of bonding CFRP and Al6061-T6 with epoxy adhesive after shot-peening treatment on the surface of Al6061-T6 specimens was proposed to improve bonding strength of a single lap joint between CFRP and Al6061-T6. More specifically, correlation between shot peening coverage on the Al6061-T6 surface and bonding strength with CFRP was experimentally analyzed. Experimental results showed that the surface roughness and the bonding strength increased as the peening time on the surface of Al6061-T6 increased up to a specific peening time (or coverage). However, the surface roughness and bonding strength decreased again under an over-peening condition of 480 seconds (300% coverage) or more. Therefore, it is necessary to search for the optimal peening time that can maximize bonding strength as well as the fatigue life of parts at a peening time between 320 (200%) and 480 s (300%) through additional experiments in future studies.