Cyclic olefin copolymer (COC) is one of the most promising optical materials; however, the brittle COC suffers from issues including a low refractive index. In this contribution, by the introduction of high refractive index comonomers including phenoxy substituted α-olefin (C 4 OAr), p-tolylthio substituted α-olefin (C 4 SAr) and carbazolyl substituted α-olefins (C 4 NAr, C 3 NAr, and C 2 NAr), the zirconocene mediated terpolymerization of ethylene (E) and tetracyclododecene (TCD) produces the preferred E-TCD-C n NAr (n = 2, 3, and 4) cyclic olefin terpolymers (COT) with tunable compositions (TCD: 11.5-35.8 mol %, C n NAr: 1.2− 5.0 mol %), high molecular weights and high glass transition temperatures (up to 167 °C) in high catalytic activities. Compared to the E-TCD copolymer (COC) material, these COT materials show the comparable thermal decomposition temperature (T d,5% = 437 °C), slightly higher strain at break value (up to 7.4%) and higher tensile strength (up to 60.5 MPa). In particular, these noncrystalline optical COT materials have significantly higher refractive indices of 1.550−1.569 and are more transparent (transmittance: 93−95%), relative to the COC materials, indicative of an excellent optical material.