Ultralong-range Rydberg trimer molecules are spectroscopically observed in an ultracold gas of Cs(nd_{3/2}) atoms. The anisotropy of the atomic Rydberg state allows for the formation of angular trimers, whose energies may not be obtained from integer multiples of dimer energies. These nonadditive trimers coexist with Rydberg dimers. The existence of such effective three-body interactions is confirmed with the observation of asymmetric line profiles and interpreted by a theoretical approach that includes relativistic spin interactions. Simulations of the observed spectra with and without angular trimer lines lend convincing support to the existence of effective three-body interactions.