A new crystalline phase (via amorphous intermediate), NCUZ-1, was obtained when MCM-41 (Si/Al β«Ψβ¬ 9) was under prolonged heating in the mother liquid (which contains NaAlO 2 , [N(CH 3 ) 4 ] 2 SiO 3 , SiO 2 , and surfactant C 16 H 33 N(CH 3 ) 3 OH(aq) at 1053C for more than two weeks. The largest d spacing of NCUZ-1 calculated from X-ray di4raction data is approx. 6 A s , indicating that the long-range order of the mesopores in MCM-41 was not present in NCUZ-1. Nitrogen absorption studies showed that NCUZ-1 contains both mesopores and micropores. The volume ratio of the mesopore to micropore is approx. 10 to 1 and the BET surface area is 400 m 2 /g. The TEM micrograph of NCUZ-1 revealed a homogenous phase with distorted mesopores. The 13 C NMR spectrum of NCUZ-1 before calcination is similar to that of uncalcined MCM-41, indicating that the organic templates in both phases have a similar structure. In the phase transformation process, the counteranion (OH Ψ ) of the surfactant template played an important role. It increased the solubility of the aluminosilicate wall; the breaking and reforming the Si+O and Al+O bonds make the phase transformation possible, although the process is very slow. When C 16 H 33 N(CH 3 ) 3 Cl, instead of C 16 H 33 N(CH 3 ) 3 OH, was used as a template, no NCUZ-1 phase was obtained under the same reaction conditions. TEM micrograph, nitrogen absorption isothermal, and 13 C NMR spectra of NCUZ-1 suggested that the mesopores were present in the NCUZ-1 phase, although there is no long-range order of these mesopores.