Crystalline form of Pregabalin characterized by X-ray powder diffraction peaks at about 5.8, 18.4, 19.2, 20.7, and 23.7° 2θ±0.2° 2θ, methods for its preparation, its pharmaceutical compositions thereof, and methods for the preparation of crystalline form of Pregabalin characterized by X-ray powder diffraction peaks at about 5.7, 15.4, 17.2, 18.2, and 23.0° 2θ±0.2° 2θ, are provided.