We provide an overview of nuclear quadrupole resonance (NQR), including two‐dimensional NQR methods and NQR imaging. We review the quantum mechanics of quadrupolar nuclear spins at zero‐field, including the trends and magnitudes of nuclear quadrupole moments. We review the coupling of these moments with the local electric field gradients, and examine the observable spectral transitions associated with this coupling.Wereview the major methods of detecting these transitions, including standard frequency‐swept NQR, SQUID detection, and field‐cycling methods. Webriefly examineNQRhardware.Weexamine multidimensional methods to obtain full quadrupolar coupling tensors and characterize exchange processes in solids, and then consider the major methods of NQR imaging. Finally, we consider computational techniques for obtaining reliable theoretical quadrupolar couplings to compare with experiment, and alert the reader tocommonpitfalls of using “canned” quantum chemistry programs and methods to calculate quadrupolar couplings.