Multiferroic laminate composites consisting of chain-end cross-linked ferroelectric polymers and magnetostrictive Metglas are reported. The composites exhibit a greatly enhanced multiferroic voltage coefficient and sensitivity relative to analogous composites. These remarkable properties are attributed to high piezoelectric and electromechanical coupling coefficients, because of the formation of larger crystalline sizes and concurrent improvement in the polarization ordering in the cross-linked polymers.