Layered double hydroxide (LDH) nanomaterials of uniform size and homogeneous distribution are successfully developed in agarose hydrogel through the electrical double migration method. To grow LDH crystals in agarose matrix, both cationic (Ni2+, Ga3+) and anionic precursors (OH- and CO32-) of LDH are simultaneously transported from solution to agarose hydrogel through electric potential, resulting in the in situ crystal growth of LDH. X-ray diffraction patterns, X-ray absorption spectra, and high-resolution transmission electron microscopic images confirm that the developed LDH is ~15 nm in size and had well-defined crystal structure. Scanning electron microscopy and small angle X-ray scattering spectroscopy showed homogeneous arrays of LDH nanocrystals along agarose sheets with homogeneous distribution. On the basis of the characterization results, we suggest that crystal nuclei are first developed on the agarose chain, and then LDHs homogeneously grow along sheets of agarose matrix.