Molecular afterglow materials with ultralong-lived excited states have attracted considerable interest owing to their promise for light-emitting devices, optical imaging, and anti-counterfeiting applications. However, the realization of ultralong afterglow emission in low-dimensional micro/nanostructures has remained an open challenge, limiting progress toward new-generation photonic applications. In this work, new types of mono/binuclear metal-organic halide micro/nanocrystals with tunable afterglow properties, made possibly by the rational control over both ultralong-lived room-temperature phosphorescence and thermally activated delayed fluorescence, are developed. Interestingly, the mono/binuclear coordination complexes present excitation-dependent luminescence across a wide range (wavelength > 150 nm) with broad emission color differences from blue to yellow owing to the multiple long-lived excited states. The 1D binuclear metal-organic microrods further exhibit excitation-dependent optical waveguide and space/time dual-resolved afterglow emission properties, endowing them with great potential in wavelength-division multiplexing information photonics and logic gates. Therefore, this work not only communicates the first example of wide-range tunable ultralong afterglow of low-dimensional metal-organic micro/nanocrystals under ambient conditions but also provides a new route to achieve optical communications and photonic logic compilation at the micro/nanoscale.