Symmetry breaking in two-dimensional layered materials plays a significant role in their macroscopic electrical, optical, magnetic and topological properties, including but not limited to spin-polarization effects, valley-contrasting physics, nonlinear Hall effects, nematic order, ferroelectricity, Bose-Einstein condensation and unconventional superconductivity. Engineering symmetry breaking of two-dimensional layered materials not only offers extraordinary opportunities to tune their physical properties, but also provides unprecedented possibilities to introduce completely new physics and technological innovations in electronics, photonics and optoelectronics. Indeed, over the past 15 years, a wide variety of physical, structural and chemical approaches have been developed to engineer symmetry breaking of two-dimensional layered materials. In this Review, we focus on the recent progresses on engineering the breaking of inversion, rotational, time reversal and spontaneous gauge symmetries in two-dimensional layered materials, and illustrate our perspectives on how these may lead to potential new physics and applications.