Infrared laser spectroscopy in helium nanodroplets is used to identify and characterize several distinct tautomers of cytosine. The experimentally observed species correspond to the lowest-energy structures obtained from ab initio calculations, also reported here. The assignment of the infrared vibrational bands in the spectra is aided by the measurement of the corresponding vibrational transition moment angles, which are also calculated using ab initio methods. In the present study we confirm the existence of three primary tautomers and provide tentative assignments for even higher-energy forms of cytosine in helium nanodroplets.