The new ethylene/cyclic olefin copolymers (COCs) are a major breakthrough in traditional polyolefins made available by metallocenes, but its high brittleness restricts the applications. Ethylene/1-octene copolymer (POE) with similar backbones is blended with COCs to compensate the rigidity of cyclic segments. Field emission scanning electron microscope photos and Raman spectra demonstrate the existence of abundant phase interfaces between POE and COC, and the phase structure changes from spherical droplets, of partial continuity to cocontinuity with rising POE components. The phase changes are considered as corresponding to the formation, expansion, and coalescence of droplets at melting state according to Van Gurp curves, Han plot, and Cole-Cole plot. Viscoelastic data show that the storage modulus, loss modulus, and complex viscosity reach a high value at medium POE contents. Furthermore, the tensile strength and fracture energy increases and then decreases, the elongation at break increases and Young's modulus reduces with the increment of POE percentage. Because of the large spherical and ellipsoidal structures and abundant interfaces, the synchronous reinforcement and toughness come true at a medium ratio of POEs. Dynamic mechanical analysis confirms the existence of the interfacial layer, and the interfacial layer becomes more pronounced with the rising POE contents exactly as the morphology and rheological findings.