The climate math is clear: carbon capture and storage (CCS) and carbon dioxide removal (CDR) must scale up to gigatons annually to mitigate climate change reach net-zero emissions and meet the Paris Agreement's goal of limiting the global temperature rise to 1.5 °C. Policy makers, business executives, investors, and the general public are beginning to see the importance of addressing climate change, and this is speeding up the implementation of CCS in many parts of the world. Numerous ongoing endeavors to capture CO2, a substantial greenhouse gas, depend on liquid chemical sorption employing strong alkaline bases or amines to reversibly bound CO2, where the sorbent is regenerated via heated desorption. In recent times, solid-state methods including silica aerogels, activated carbon, and amine sorbents attached to supports have become relevant. Both categories of CO2 collecting technologies have challenges related to selectivity, water rejection, energy consumption, transport limitations, and longevity. As part of the worldwide CCS and CDR endeavor, we aim to design long-lasting, efficient, and subsequently industrially developable carbon capture system for post-combustion capture (PCC) and atmospheric direct air capture (DAC) of CO2. This work explores novel modifications to foundational metal-organic frameworks (MOFs), particularly UiO-66, along with its applications to PCC and DAC. This work is also focused on development of a novel method to encapsulate these MOFs in composite nanofibrous membranes leading to superior CO2 capture capacities (over 1 mmol/g of sorbent) and simplistic reversibility. This would be achieved by tailoring the chemistry, hydrophobicity, porosity, and morphology of highly loaded amine-based metal organic framework/porous organic polymer composite nanofibers (such as UiO-66/PIM-1), using facile synthesis and gas-assisted electrospinning.