The performance of an adsorption-based separation process is dictated by the choices of the adsorbent and the process configuration. In typical studies, either several materials are screened for a specific process configuration to find the best candidate, or the performance of several process configurations is evaluated for a specific material. However, it has long been suggested that to truly maximize the potential of a given material, it should be “married” to processes. Here, we have developed a modeling framework for a hybrid adsorption cycle composed of several process configurations and a unified optimization approach to select the optimal material-process combination. We have shown through several case studies that (1) one needs to employ an integrated optimization approach to maximize the potential of any material when screening for a given application; (2) one should not generalize the observations regarding the best process configuration from one material to every other material.