A novel approach for integrated adsorbent and process design is proposed. The traditional pressure or vacuum swing adsorption (PSA) / vacuum swing adsorption (VSA) process optimization for chosen objectives, where operating conditions are the decision variables, and CO2 purity and recovery are constraints, is expanded to include adsorbent isotherm characteristics as additional decision variables. Two VSA cycles, namely a four-step process(1), currently known to have the lowest energy consumption for CO2 capture and concentration (CCC), and a six-step process(2), recently proven to have a wider operating window for the evacuation pressure, have been investigated in the current study. The integrated optimization results simultaneously provide the lower bound of minimum energy and upper bound of maximum productivity for CCC achievable from the two VSA processes along with the operating conditions and the corresponding isotherm shapes necessary to achieve them. It may be viewed as an enabler for adsorbent design or expedient adsorbent search by process inversion. (c) 2017 American Institute of Chemical Engineers AIChE J, 63: 2987-2995, 2017