Following recent advances in the growing field of nanotechnology, nanomaterials can be designed as superior sensitive nanosensors. However, the development of selective and efficient signaling systems for the detection and removal of various chemically and biologically pertinent species has received a great deal of interest. A simple design with fast, reversible, sensitive, selective, inexpensive, and specific recognition of toxic ions is needed in chemosensor technology. Significantly, the interaction between the target species and nanomaterial with suitable functionality is designed to produce a physicochemical perturbation on the chemosensor that can be converted into a measurable effect, such as an optical or electrical signal. The functionalized ordered porous carriers have unique properties that offer a significant advantage for the selective removal and sensitive detection of target species. In this manuscript, we designed optical chemical supermicrosensors for Cu(II) ions based on two- and three-dimensional (2D and 3D), hexagonal and cubic Fd3m supermicroporous aluminosilica monoliths as selective shape and size carriers. The key advantage of 3D cubic Fd3m supermicropores is the easy access to target ions, such as ion transports, and high affinity responses of the receptor-metal analyte binding events, resulting in the easy generation and transduction of optical color signals even at a trace level of Cu(II) target ions. Such an aluminosilica supermicrosensor design enables sensitive recognition of Cu(II) ions up to nanomolar concentrations (∼10−9mol/dm3) with rapid response time (in the order of seconds). The 3D cubic Fd3m supermicrosensors also exhibited easy accessibility of target ions, such as ion transports; and high affinity binding events, particularly at a trace level of target ions. Moreover, these designs with suitable accommodation exhibit long-term stability and create revisable sensing systems with multiple regeneration/reuse cycles. However, the sensing system recovery is very simple and can be achieved via ClO4− anion treatment. The key results in this manuscript is the exhibition of the ion-selective determination in real matrix of the optical supermicrosensors based on 2D and 3D ordered supermicroporous aluminosilica monoliths, despite the presence of competitive species. This manuscript provides a basis for further development in chemosensor technology.