The development of more efficient processes for CO~2~ capture from the flue streams of power plants is considered a key to the reduction of greenhouse gas emissions implicated in global warming. Indeed, several U.S. and international climate change initiatives have identified the urgent need for improved materials and methods for CO~2~ capture. Conventional CO~2~ capture processes employed in power plants world-wide are typically postcombustion βwet scrubbingβ methods involving the absorption of CO~2~ by amine-containing solvents such as methanolamine (MEA). These present several disadvantages, including the considerable heat required in regeneration of the solvent and the necessary use of inhibitors for corrosion control, which lead to reduced efficiencies and increased costs for electricity production. This perspective article seeks to highlight the most recent advances in new materials for CO~2~ capture from power plant flue streams, with particular emphasis on the rapidly expanding field of metalβorganic frameworks. Ultimately, the development of new classes of efficient, cost-effective, and industrially viable capture materials for application in carbon capture and storage (CCS) systems offers an immense opportunity to reduce atmospheric emissions of greenhouse gases on a national and international scale.