<p>The ¹⁴N nuclear quadrupole resonance (NQR) spectrum of nitrourea has been recorded using Cross Relaxation Double Resonance. Nitrourea is an important reagent and intermediate in many organic chemical reactions and has applications in the preparation of medicines, explosives, foaming reagents and manyadditives. It has three distinct nitrogen atoms in its chemical structure. One nitrogen atom belongs to the nitro group while the other two are part of the urea moiety (carbamide). The ¹⁴N NQR experimental quadrupole coupling constants (χ) and asymmetry parameters (η) of nitrourea, determined from the ¹⁴N NQR cross relaxation spectrum, have been compared to its calculated ab-initio values and the orientation of the principal electric field gradient (EFG) axes for each nitrogen atom has been assigned. The nitrogen atom of the nitro group has the lowest calculated quadrupole coupling constant (χ) and by extension lowest q_zz EFG component while the nitramine nitrogen attached to the nitro group has the largest quadrupole constant (χ) and asymmetry parameter (η). The asymmetry parameters (η) and quadrupole coupling constants (χ) for the nitrogen atoms support the presence of intermolecular hydrogen bonding in the molecule.</p>