The high resolution rotational spectroscopic observation of 1,1-diiodoethane is investigated using a pulsed jet, cavity Fourier transform microwave (FTMW) spectrometer over the frequency range 11.5–18 GHz for the first time. The rotational constants, the centrifugal distortion constants, the nuclear spin-rotation coupling constants, and the complete tensor components of the nuclear quadrupole coupling for both iodine nuclei have been determined and reported. The fitted rotational constants are A = 4548.320446(47), B = 625.629141(55), C = 558.798939(43) MHz and the nuclear quadrupole coupling constants are χ_aa = −1089.8125(7), χ_bb − χ_cc = −542.3162(13), |χ_ab| = 1215.7505(10), χ_bc = 340.8983(14), and |χ_ac| = 562.4206(19) MHz. No A-E splittings due to the methyl group internal rotation were observed. Many dipole-forbidden/electric quadrupole coupling allowed transitions were observed in the spectrum due to the large iodine quadrupole coupling effect. Quantum chemical calculations were performed at the CCSD(T)/aug-cc-pVTZ-pp level of theory. The calculated rotational constants, centrifugal distortion constants, and hyperfine constants were used to guide the data analysis.