The absorption of CO2 on MgO is being studied in depth in order to enhance carbon engineering. Production of carbonate on MgO surfaces, such as MgCO3, for example, has been shown to hinder further carbon lattice transit and lower CO2 collecting efficiency. To avoid the carbonate blocking effect, we mimic the water harvesting nano-surface systems of desert beetles, which use alternate hydrophobic and hydrophilic surface domains to collect liquid water and convey condensed droplets down to their mouths, respectively. We made CO2-philic MgO and CO2-phobic Mg(OH)2 nanocomposites from electrospun nano-MgO by vapor steaming for 2–20 min at 100 °C. The crystal structure, morphology, and surface properties of the produced samples were instrumentally characterized using XRD, SEM, XPS, BET, and TGA. We observed that (1) fiber morphology shifted from hierarchical particle and sheet-like structures to flower-like structures, and (2) CO2 capture capacity shifted by around 25%. As a result, the carbonate production and breakdown processes may be managed and improved using vapor steaming technology. These findings point to a new CO2 absorption technique and technology that might pave the way for more CO2 capture, mineralization, and fuel synthesis options.