We review the techniques, applications, characteristics, and insights gained from the use of theoretical calculations that were applied to the study of layer double hydroxides (LDHs) materials by using a series of typical case studies. The advantages and shortcomings of different theoretical calculation methods (quantum mechanics, molecular mechanics, geometric model, and electrostatic potential energy model) for the study of the properties of LDHs minerals are compared. Based on quantum mechanics calculations, we obtained information about template effects on the construction of layered double hydroxides, super molecular interactions in LDHs containing simple anions, electronic properties, and reaction pathways etc. Compared with quantum mechanics, molecular mechanics is quicker in obtaining information about the interlayer structure, arrangement, orientation, hydration, and the swelling trajectory as well as elastic constants etc of LDHs intercalated with various anions. The geometric model and electrostatic potential energy model offer a more intuitive and visual mathematical model of LDHs minerals. The calculations were done on the verge of full size LDHs, which may allow the prediction of the crystal structure. Along with the development of theoretical methods and computer techniques, computational simulation method has become an effective adjust to experimental techniques for obtaining the microscopic structures, electronic and dynamic properties of LDHs minerals.