The adsorption and dynamical behavior of the muonated cyclohexadienyl radical (C(6)H(6)Mu) in NaY zeolite, formed by muonium (Mu) addition on adsorbed benzene. was investigated by the muon spin resonance (muSR) technique, primarily at loadings of 2-3 C6H6 molecules per supercage of NaY. The dynamics of this radical are expected to be the same as its isotopic analogue, C6H7, for which there are no similar data available. Both TF-muSR and ALC-muSR spectra were recorded, with the most detailed information provided by the positions and line widths of the avoided level crossing resonances. In concert with H-2 NMR, neutron diffraction and molecular dynamics studies of the parent benzene molecule, as well as current theoretical calculations, the dominant adsorption site for the C(6)H(6)Mu radical is believed to be the S-II Na cation, within a supercage, which gives rise to three observed ALC lines, corresponding to two different orientations for the muon (proton) of the CHMu methylene group: pointing toward (endo) and away (exo) from the Na cation. The cation interaction gives rise to unprecedentedly large (approximate to20%) shifts in hyperfine coupling constants, indicative of a strong bond formed with the T electrons of the C(6)H(6)Mu radical. An additional but weaker resonance line is also seen, which is interpreted as being due to adsorption at the window sites between supercages. The ALC lines associated with the CH,,Mu radical bound to both the Na cation and window sites are all broad, approximate to1 kG, change little with temperature and exhibit mainly static line shapes over the whole temperature range studied, from 3 to 322 K. This indicates a much stronger host-guest interaction for C(6)H(6)Mu, particularly with the Na cation. than is known for benzene, to the extent that this site acts as an effective trap for the free radical, over the critical muSR time scale of 50 ns.