The invention provides a method of readily manufacturing a lithium secondary battery including a solid electrolyte layer having space for accommodating deposited lithium. A lithium secondary battery includes a positive electrode element, a negative electrode element and a solid electrolyte layer placed between them. A method of manufacturing the battery includes a first step of stacking at least a first group of particles and a second group of particles to form the solid electrolyte layer, the second group of particles having an average particle diameter larger than that of the first group of particles, and a second step of stacking the positive and negative electrode elements on the solid electrolyte layer such that the negative electrode element is in contact with a surface of the second group of particles in the solid electrolyte layer.