In this paper, a series of pure Ni 1−x Zn x Fe 2 O 4 (0≤x≤1) spinel ferrites have been synthesized successfully using a novel route through calcination of tailored hydrotalcite-like layered double hydroxide molecular precursors of the type [(Ni+Zn) 1−x−y Fe y 2+ Fe x 3+ (OH) 2 ] x+ (SO 4 2− ) x/2 ·mH 2 O at 900°C for 2h, in which the molar ratio of (Ni 2+ +Zn 2+ )/(Fe 2+ +Fe 3+ ) was adjusted to the same value as that in single spinel ferrite itself. The physico-chemical characteristics of the LDHs and their resulting calcined products were investigated by powder X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS) and Mössbauer spectroscopy. The results indicate that calcination of the as-synthesized LDH precursor affords a pure single Ni 1−x Zn x Fe 2 O 4 (0≤x≤1) spinel ferrite phase. Moreover, formation of pure ferrites starting from LDHs precursors requires a much lower temperature and shorter time, leading to a lower chance of side-reactions occurring, because all metal cations on the brucite-like layers of LDHs can be uniformly distributed at an atomic level.