The manipulation of the strain-mediated magnetoelectric (ME) coupling strength is investigated by inserting a thin Ti layer (0–10 nm) between a 50 nm Co50Fe50 layer and a (011) oriented lead magnesium niobate-lead titanate (PMN-PT) substrate. A record high remanence ratio (Mr/Ms) tunability of 100% has been demonstrated in the 50 nm CoFe/8 nm Ti/PMN-PT heterostructure, when a total in-plane piezoelectric strain of −1821 ppm was applied at an electric field (E-field) of 16 kV/cm. The ME coupling strength is gradually optimized as the Ti layer thickness increases. Magnetic energy calculation showed that with increasing Ti layer thickness the uniaxial magnetic anisotropy energy (Euni) was reduced from 43 ± 1 kJ/m3 to 29.8 ± 1 kJ/m3. The reduction of Euni makes the strain effect dominant in the total magnetic energy, thus gives an obvious enhanced ME coupling strength.