The goal of producing polyetheretherketone/polyetherimide (PEEK/PEI) blends is to combine the outstanding properties that both polymers present separately. Despite being miscible polymers, it is possible to achieve PEEK/PEI multilayered blends in which PEEK crystallinity is not significantly inhibited, as opposed to conventional extruding processes that lead to homogeneous mixtures with total polymer chain interpenetration. This study investigated a 50/50 (volume fraction) PEEK/PEI multilayered polymer blend in which manufacturing parameters were tailored to simultaneously achieve PEEK–PEI adhesion while keeping PEEK crystallinity in order to optimize the mechanical properties of this heterogeneous polymer blend. The interface adhesion was characterized with the use of three-point bending tests, which proved that a processing temperature below the melting point of PEEK produced weak PEEK–PEI interfaces. Results from differential scanning calorimetry (DSC), dynamic mechanical analysis (DMA), and X-ray diffraction analysis (XRD) showed that under a 350 °C consolidation temperature, there is a partial mixing of PEEK and PEI layers in the interface that provides good adhesion. The thickness of the mixed homogeneous region at this temperature exhibits reduced sensitivity to processing time, which ensures that both polymers essentially remain separate phases. This also entails that multilayered blends with good mechanical properties can be reliably produced with short manufacturing cycles. The combination of mechanical performance and potential joining capability supports their use in a wide range of applications in the automotive, marine, and aerospace industries.