Microporous silica membranes have shown promise as potential candidates for energy-efficient chemical separation. Herein, we report the ultrafast synthesis of silica membranes, on the order of minutes, in atmospheric-pressure, low-temperature plasma. Direct deposition in the discharge region of atmospheric-pressure plasma enables the immediate formation of a thin silica layer on a porous substrate. The plasma-deposited layer had a thickness of similar to 13 nm and was confined to the immediate surface of the substrate. With an increase in deposition temperature, we observed an increase in the inorganic nature of the plasma-deposited layer and simultaneous improvement in the membrane performance. Consequently, the resulting membranes exhibited outstanding permeance for small-sized gas molecules, such as H-2 (>10(-6) mol m(-2) s(-1) pa(-1)) with a high H-2/SF6 permeance ratio of similar to 6300, providing a nonthermal alternative for the fabrication of silica-based membranes.