The joining of composites can be performed in an extremely short time with more energy-efficient ultrasonic welding techniques. The current research investigated the performance optimization of ultrasonic welding of carbon/Elium® composite to carbon/epoxy composite using a polymethyl methacrylate (PMMA) coupling interlayer. The weld strength was quantified by static lap shear strength (LSS) testing. A new methodology was used by creating a PMMA coupling layer on the epoxy composite adherend to achieve an improved interphase and thus enhance the weld properties. The LSS of Elium (EL)-Epoxy (EP) _0.25_0.25 was found to be 190% higher compared to that of EL-EP, confirming the effectiveness of the strategy used for creating an interlayer thermoplastic coupling layer. The time required for welding was optimized to be 2s as compared to 10 min required for adhesive bonding. Scanning electron microscopic images of epoxy and PMMA/Elium matrix interphase were observed to have a rough surface and remained largely unaffected by welding. There was an interphase change further away from the interphase to a rougher texture. There was little to no effect on the penultimate layer on the weld strength, as no interphase change could be observed after welding. Fractography investigation revealed shear cusps, matrix plastic deformation, fiber imprints, fiber pull-out, and good adhesion between matrix and fiber, features seen for configuration with maximum LSS. The current research findings present a way to join Elium® with epoxy composites that could be used in applications that require a selective strengthening, such as in sporting goods and consumer products. Furthermore, a detailed investigation is ongoing to use different filler particles and coupling layers to reach the maximum welding performance.