Titan, the largest satellite of Saturn, possesses a dense N2-CH4 atmosphere rich in organics with a complex chemistry that could be similar to Earth's primordial atmosphere. Due to its massive atmosphere and the long distance to the Sun, cosmic rays are the main energetic source of the lower part of the atmosphere. Cosmic radiation can reach Titan's troposphere (z < 40 km) and activate the chemistry at depths where UV light and high-energy electrons cannot penetrate. The interaction of cosmic rays with the neutral constituents of Titan produces a complex ion chemistry that leads to the formation of a high variety of massive ions and organic molecules. The low temperatures and high pressures prevailing in Titan's atmosphere result in a high efficiency of three-body reactions and on the formation of ion clusters. Association of neutral molecules with HCNH+, CH3CNH+, and HC3NH+ produces ions containing the CN group, and the electron recombination of these clusters can produce a high variety of N-containing compounds. Here we propose schemes to synthesize nitrile-type molecules from the dissociative recombination ion clusters produced by cosmic rays. Our ion chemistry model can explain the existence of some of the nitriles found in laboratory studies, such as propenenitrile, propanenitrile, butanenitrile, pentanenitrile, and 10 more as well as predict the existence of new species. Experimental simulations of Titan's atmosphere yield the formation of a high number of species, which are not considered in the chemical schemes of current photochemical models.