A series of green poly(isoprene-co-myrcene) (PIMy) elastomers were designed and prepared by coordination polymerization to solve the fossil shortage and achieve an excellent low-temperature resistance property. The properties of PIMy could be tailored upon varying the comonomer feed ratios. The structure and thermal stability were investigated by NMR, differential scanning calorimetry (DSC), and thermogravimetric analysis (TGA) analyses. The cis-1,4 structure content of PIMy exceeded 95%, and the Tg of PIMy was below −60 °C without crystallization at low temperatures. With the increase of myrcene content, the tensile strength of PIMy/silica nanocomposites decreased, the wet skid resistance was improved, and PIMy with myrcene content of 5–20 mol % had better comprehensive properties. The introduction of PIMy in solution-polymerized styrene–butadiene rubber (SSBR) increased the tan δ value at −20 °C and improved the ice skid resistance performance. The Laboratory Abrasion Tester (LAT-100) test results showed that the addition of PIMy significantly improved the friction of SSBR on the ice surface with a maximum improvement of 161%. The PIMy prepared in this study is expected to be used in low-temperature-resistant rubber products such as seals and winter tires.