In this study, we develop a novel one-step method for synthesis of nickel oxide/silicon dioxide (NiO/SiO(2)) mesoporous composites by using N-hexadecyl ethylenediamine triacetate (HED3A) as structure-directing agent. Besides playing a role in directing the mesophase formation, the anionic surfactant also functions as a chelating agent that binds nickel ions. Ultraviolet-visible (UV-vis) and Fourier transform infrared (FTIR) spectroscopic analyses were undertaken to determine the chelating ability between HED3A and nickel ions. By adjusting the molar ratio of Ni(2+)/HED3A in the template solution, a series of mesoporous composites with various NiO contents were obtained after calcination. These composites were characterized by X-ray diffraction (XRD), high resolution transmission electron microscopy (HRTEM), and nitrogen adsorption/desorption. The results showed that the generated NiO nanoparticles were aggregated into clusters with the size less than 20 nm, and the composites retained mesoporous characteristics even with high NiO contents. HRTEM images also revealed the migration and aggregation for NiO nanoparticles during the sintering process. Moreover, the energy-dispersive X-ray spectrum (EDX) results showed a close linear relationship between Ni/Si in the composites and Ni(2+)/HED3A in the templates. This chelating surfactant-assistant encapsulation route has the potential to synthesize diversiform metal oxide/silica mesoporous composites with designated compositions. (C) 2011 Elsevier Inc. All rights reserved.