In this study, an innovative nonpolar nanoporous AlN growth technology was successfully developed, which realized in situ nitrided growth of nonpolar AlN by γ-LiAlO 2 (LAO) crystals through the crystal elements expelled and recrystallization (CEER) method. In this way, we can effectively avoid the quantum-confined Stark effect by the growth of nonpolar AlN, paving the way for the fabrication of high quantum efficiency AlN-based optoelectronic devices. The prepared AlN crystalline was fully characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), Raman spectroscopy, and X-ray photoelectron spectroscopy (XPS). The pore structure has an average pore size of about 40−50 nm, making it a great potential as a patterned substrate for epitaxial lateral overgrowth and a template for GaN-based LED devices. The rocking curve of XRD shows a full width at half-maximum (fwhm) of 0.75°, indicating relatively good crystalline quality. The phonon frequency of the E 2 (high) phonon mode in the Raman spectrum is shifted to 657.7 cm −1 , which is slightly blueshifted compared with the E 2 (high) phonon mode of the ideal AlN crystal, reflecting the slight compressive stress in the crystal structure. In addition, the AlN crystal observed by TEM has a depth of more than 4 μm, further confirming the uniformity of the crystal and the excellent three-dimensional connectivity of the pore structure. The TEM images also show that the AlN crystalline prepared by the CEER method has a lower defect density, which is conducive to greatly improving the performance of AlN-based devices. This technique enables a novel approach to synthesizing a-plane AlN, a significant advancement for the production of highquality nonpolar AlN materials and the development of nonpolar LEDs.