A series of monodisperse cruciate multilayer H3Sr6(PO4)(5)center dot 2H(2)O:Eu2+ microarchitectures assembled by crossed nanorods have been successfully synthesized via a facile surfactant-assisted hydrothermal route. XRD and FT-IR confirmed the existence of crystalline water in the phosphor. The FE-SEM images revealed that the phase and morphology of resulting samples were strongly depended on the optimization of the reaction conditions, especially the pH value and the molar ratio of citric acid (CA)/Cations. Furthermore, the possible growth mechanism of H3Sr6(PO4)(5)center dot 2H(2)O:Eu2+ microarchitectures was proposed in detail. Under near-ultraviolet excitation of 365 nm, the as-obtained H3Sr6(PO4)(5)center dot 2H(2)O:0.05Eu(2+) sample exhibited intense wide characteristic blue emission of Eu2+, which could be decomposed by Gaussian fitting into two peaks corresponding to different Eu2+ luminous centers. The present results demonstrated that the morphology-tunable H3Sr6(PO4)(5)center dot 2H(2)O:Eu2+ microarchitecture could be used as a potential candidate for future optoelectronic device applications.