The di electric pt"Oper t ies of polyc hlorotrifluoroethylene ( '1' m= 224°C, T g = 52°C) h ave been meas ured at temperatures between -50 and + 250 °C, and at frequ encies between 0.1 cis a nd 8.6 kMc/s. Specim ens of known crystallinit ies, ra nging from x = 0.80 to x = O.OO (pure liquid) were studied . Co mpre hens ive ta bles of data a rc prese nted. The experimental techniques e mplo.ved to measure the dielectric properties over these wide r'anges of temperature, fr equency, phys ical sta te, and sa mple type (di s ks, cylinders, and t hin film s), are disc ussed. The operation a nd calibrat ion of the s pecimen holder, bridges, r eson a nt circuits, a nd waveg uide a ppamt us used are di scussed in detail.When t he dielectric loss index, , ", at 1 cis is plotted as a fun ction of temperature for a hig hly crystallin e sp ecimen (x = 0.80), where the crystallini ty co ns ists la rgely of la mellar spheruli tes, Llu-ee distin ct loss peaks a re readily a pparent. These peaks occ ur at abo ut -40°C (low-te mperaL ure process), 95°C (i nterm edi ate-Le mperat ure process), and 150°C (hig h-temperature pt'ocess) . The di electri c data a re co mpa red with t he m ec ha ni cal loss data obtained at 1 cis by McCrum. Mech a nical loss p caks at temp eratures vir t ua lly iden t ical to Lhose in t he , " ve r~u s T plot a re fo und .Th e high-tempemtuTe process is attri b uted to the presence of well-form ed cha in-folded lamella r sph erulites. Some ev idence poin ts to the surfaces of t he la mellae as the site of the loss}mec ha nis m. The high-temperature loss peak docs no t a ppear in resol ved form in n011-spheruli t ic s peci mens even when the cr ystalli nity is hi gh. The intermediate-tem pemture process or'igin 'ttes in the norm al s upe rcooled a morp ho us phase, a nd is du e to t he co mplex dipol e relaxatio n effects involving mot ions of la rge numbers of poly mer cha in seg me nts t hat a re assoc iated wi th t he onset of the glass transition at T g = .52 °C. As de termined by i7 -T da.ta, the glass trnns it ion te mpemture at T g = 52°C t hat is associated wi t ll t his r elaxation eff ect docs not s hift appreciably wit h increas ing crys tallini ty. The low-tem perature dielecLri e loss process, wh ich is acL ive fa r belo w T " or igin ntes principa lly in t Ile s up ercooled a morphous regions, and ev iden t ly corres ponds to a fa irly simple motion invo lvin g a s mall number of cha in segments. This process t ends to ex hibi t a noma lous behavior in h ig hly crystalline s pecimens, pctrLicula.rly at 101V te mperatures.A la rge dipo la r contribu t ion of the crys tals to the static di electric cons tan t was obser ved. This co nLribu t ion increased with in creas in g temperature, an d co r respo nded to a very r a pid dipole reori e ntation process ( T~10-rr sec at 23°C).