Novel NO absorbent–releaser is discovered by utilizing the as-synthesized mesoporous silica MCM-41 or MCM-48, not only saving the energy and time for removal of template, but also establishing the way to utilize the micelles for new applications of health care. The micelles of cetyltrimethylammonium bromide (CTAB) in the as-synthesized MCM-48 or MCM-41 have a configuration of spoke-like in the wheel or net-like inside the channel, intercepting and capturing the NO in gas flow with an unwonted high absorption capacity. Once NO is absorbed on these composites, it forms surface nitrous species and nitrates that are stable in atmosphere, achieving the storage of NO in ambient environment. Finally, the NO can be acid-triggered released in the solution with the pH value same as that of the gastric juice, providing a new low-cost candidate for delivering exogenous NO. Various factors, including surfactant types, framework structures, and absorption temperatures, are investigated to expatiate this new controllable absorption–release process, exploiting further the utilization of micelles and affording a new application of as-synthesized mesoporous material in the drug delivery system.