Despite intensive research and development efforts in renewable energy in recent years, more than 80% of the energy supply in the year 2040 is expected to come from fossil fuel-based sources. Increasing anthropogenic greenhouse gas emissions led the United States to legislatively limit domestic CO2 emissions to between 1000-1100 lb/MWh for new fossil fuel-fired power plants, thus creating an urgent need for efficient gas separation (capture) processes. Meanwhile, the gradual replacement of coal with cleaner burning natural gas will introduce additional challenges of its own since nearly 40% of the world's gas reserves are sour due to high concentrations of corrosive and toxic H2S and CO2 gases, both of which are to be separated. Next-generation micro-structured reactors for industrial mass and heat transfer processes are a disruptive technology that could yield substantial process intensification, size reduction, increased process control and safety. This dissertation proposes a transformative gas separation solution utilizing advanced micro-structured surfaces and gas delivery manifolds that serves to enhance gas separation processes. Experimental and numerical approaches have been used to achieve aggressive enhancements for a solvent-based CO2 absorption process. A laboratory-scale microreactor was investigated to fundamentally understand the physics of multiphase fluid flow with chemical reactions at the length scales under consideration. Reactor design parameters that promote rapid gas separation were studied. Computational fluid dynamics was used to develop inexpensive stationary (fixed) interface models for incorporation with optimization engines, as well as high fidelity unsteady (deforming) interface models featuring universal flow regime predictive capabilities. Scalability was investigated by developing a multiport microreactor and a stacked multiport microreactor that represented one and two orders magnitude increase in throughput, respectively. The present reactors achieved mass transfer coefficients as high as 400 1/s, which is between 2-4 orders of magnitude higher than conventional gas separation technologies and can be attributed to the impressive interfacial contact areas as high as 15,000 m2/m3 realized in this study through innovative design of the system. The substantial enhancement in performance achieved is indicative of the high level of process intensification that can be attained using the proposed micro-structured reactors for gas separation processes for diverse energy engineering applications. This dissertation is the first comprehensive work on the application of micro-structured surfaces and fluid delivery systems for gas separation and gas sweetening applications. More than ten refereed technical publications have resulted from this work, part of which has already been widely received by the community.